RU2790204C2 - In situ production and functionalization of carbon materials through gas-liquid mass transfer and its use - Google Patents

Abstract

FIELD: chemistry.

SUBSTANCE: inventions relate to the production of carbon material and its use. A method for the production of solid carbon material is described, including: delivery of liquid containing at least one liquid organic compound to a reaction zone of a reactor; delivery of gas containing at least one gaseous organic compound to the reaction zone of the reactor; and induction of a chemical reaction including gas-liquid mass transfer between at least one liquid organic compound and at least one gaseous organic compound. In this case, the chemical reaction occurs in the reaction zone of the reactor; solid carbon material is obtained by reaction; solid carbon material is obtained during the reaction in the form of a dispersion including solid carbon material dispersed in liquid; the chemical reaction is a homogeneous reaction including homogeneous nucleation of solid carbon material in the reaction zone of the reactor; the chemical reaction does not occur on or in a catalyst; and the resulting solid carbon material is selected from a group containing graphite, expanded graphite, graphite-like material, graphene, graphene-like material, carbon plates, carbon nanotubes, carbon bulbs, other carbon allotrope, composite containing graphene, cationic graphene, or any combination thereof. A dispersion obtained by the above-mentioned method is described. The use of solid carbon material obtained by the above-described method as part of a battery anode, battery cathode, conductive material, heat-conducting material, lubricating fluid, or heat-conducting fluid is described. The use of a dispersion obtained by the above-described method to obtain a part of a battery anode, battery cathode, conductive material, heat-conducting material, lubricating fluid, or heat-conducting fluid is described.

EFFECT: production of carbon material.

37 cl, 43 dwg, 10 tbl, 14 ex

Description

CROSS-REFERENCE TO RELATED APPLICATIONS

This application claims priority to U.S. Provisional Application No. 62/783,713, filed December 21, 2018, and U.S. Provisional Application No. 62/926,283, filed October 25, 2019, each of which is incorporated herein by reference in its entirety.

BACKGROUND OF THE INVENTION

Graphene is used in a wide range of applications, including anti-corrosion coatings and paints, electronics, solar panels, drug delivery, batteries, and water filters. However, a significant problem in the commercialization of graphene is the lack of reliable mass production methods for the production of low cost, high quality graphene. The various ways of producing graphene can be classified into top-down and bottom-up approaches. For example, conventional top-down methods include: (i) chemically converted graphene (graphene oxide reduction), (ii) electrochemical exfoliation, and (iii) liquid phase exfoliation (LPE) in the presence or absence of surfactants. Bottom-up approaches include: (i) graphene structures synthesized from low molecular weight organic precursors by catalytic chemical vapor deposition (CVD), (ii) organic synthesis, and (iii) epitaxial growth on SiC or other substrates.

Among these methods, top-down chemical reduction of exfoliated graphene oxide (GO) is perhaps the most common strategy for large-scale production of graphene. This method corresponds to the chemical transformation of graphite. The process is very long (eg, approximately 5 hours), typically requires the use of expensive harmful chemicals such as sulfuric acid, nitric acid, and potassium permanganate, and intense energy (eg, requires high temperatures ranging from 800°C to 1050 °C). Also, the process is inefficient. Strong acids consume as much as 20-50% of seed graphite. The process requires lengthy washing and cleaning steps, which produces huge amounts of wastewater that must be treated accordingly. GO crystals require further chemical reduction to reduce the oxygen content. This reduction leads to a reduction in graphene oxide (rGO). The recovery procedure usually involves the further use of pesticides such as hydrazine. Even after restoration, graphene is far from being intact. Post-production methods for reducing GO to rGO do not completely remove the oxygen introduced by the high oxidation process. The remaining oxygen groups can be considered a form of chemical defects. In addition, the removal of oxygen typically results in the formation of physical defects in the form of voids and damage to the edges.

Most of the above processes do not create pristine (i.e. pure) graphene. Intact graphene is a monomolecular layer or a small number of layers of graphene plates that do not have chemical and physical defects. Both of these defects degrade the unique thermal properties required for heat transfer as well as the electrical properties required in microelectronics and energy storage. Typical chemical defects are oxygen functional groups located on the surface or edges of graphene plates, which significantly reduces the thermal conductivity of graphene. For example, even 5% oxygen will reduce the thermal conductivity of graphene by 95% (eg, see Xin Mu et al., Sci. Reports , 4: 3909; DOI: 10.1038/srep03909). Chemical defects also reduce the electrical conductivity of graphene. GO with no more than 35% oxygen acts as an insulator rather than a conductor. Physical defects include holes and voids on the plane and edges of graphene plates. These holes and voids prevent the free flow of heat and electrons through the graphene plane. Physical defects are often created during the production or removal of oxygen.

Another major problem associated with working with graphene is that it is very difficult to create stable graphene dispersions. Graphene is a solid that is insoluble in solvent, so graphene is used in powder form or as a dispersion. There are many problems associated with trying to create dispersions containing graphene, including multi-stage processes with increased waste and costs. See, for example, Liang et al., Coatings , 2018, 8, 33; Dong et al., Nature Communications, January 8, 2018, 9, article number 76; and Johnson, Current Opinion in Colloid & Interface Science , 2015, 20(5-6), 367-382.

Thus, there is a need for methods that address these and other problems associated with the creation of graphene and other carbon materials. This document presents such methods for producing carbon materials, as well as methods for the functionalization of materials, which can give graphene, including pure graphene, and can be scalable, short-term and reduce production costs compared to conventional approaches.

SUMMARY OF THE INVENTION

The invention relates to methods for producing hard carbon materials and functionalization of materials such as hard carbon materials, in particular graphene. These methods include obtaining solid carbon materials in a liquid in situ, obtaining a dispersion of solid carbon material, which in some embodiments, the implementation is considered stable dispersions. The invention also relates to the uses and applications of the carbon material(s).

The methods described herein for producing a solid carbon material, wherein the method includes delivering a liquid containing at least one liquid organic compound to a reaction zone of a reactor; delivering a gas containing at least one gaseous organic compound to the reaction zone of the reactor; and inducing a chemical reaction between at least one liquid organic compound and at least one gaseous organic compound, where: the chemical reaction occurs in the reaction zone of the reactor; solid carbon material is obtained by the reaction; the solid carbon material is obtained during the reaction in the form of a dispersion containing the solid carbon material dispersed in a liquid; and the chemical reaction is a homogeneous reaction involving homogeneous nucleation of solid carbon material in the reaction zone of the reactor. Preferably, the chemical reaction involves gas-liquid mass transfer. Preferably, but not necessarily, the gas composition is different from the liquid composition. Preferably, but not necessarily, the composition of the at least one gaseous compound is different from the composition of the at least one liquid organic compound. Optionally, the chemical reaction does not occur on or with the catalyst. Preferably, but not necessarily, the method does not include heterogeneous nucleation of a solid carbon material on a solid support. Optionally, a liquid delivery step is performed via the first inlet stream to the reaction zone, and a gas delivery step is performed via the second inlet stream to the reaction zone; where the paths of the first stream and the second input stream are different and are physically separate. Optionally, the liquid delivery step and the gas delivery step are performed simultaneously. Optionally, the gas delivery step is performed after the liquid is delivered to the reaction zone. Preferably, the solid carbon material remains dispersed in the liquid while present in the reaction zone. Preferably, but not necessarily, the liquid is substantially free of solid carbon material during the liquid delivery stage and prior to the gas delivery and chemical reaction induction stages. Preferably, but not necessarily, the liquid is substantially free of solids and is not substantially colloidal, slurry or sol during the liquid delivery stage and up to the gas delivery and chemical reaction induction stages. Preferably, but not necessarily, the solid carbon material is formed only in the reaction zone of the reactor. Optionally, no solid carbon material is obtained if the process is performed without a gas delivery step under otherwise equivalent steps and conditions. Preferably, but not necessarily, gas delivery includes gas capture, gas injection, or a combination of both. Optionally, the gas is entrained in the pressurized liquid, the gas is injected into the liquid, or the gas is bubbled into the liquid, or a combination of these methods. Preferably, the gas is delivered directly to the reaction zone during the gas delivery step. Preferably, but not necessarily, the gas delivery and chemical reaction induction steps are performed simultaneously or substantially simultaneously (e.g., within 5 minutes, within 4 minutes, within 2 minutes, within 1 minute, within 30 seconds, within 15 seconds , within 10 seconds, within 5 seconds, or within 1 second). Preferably, at least one liquid organic compound and at least one gaseous organic compound at the same time (for example, within 5 minutes, within 4 minutes, within 2 minutes, within 1 minute, within 30 seconds, within within 15 seconds, within 10 seconds, within 5 seconds, or within 1 second) are present in the reaction zone. Optionally, the step of inducing a chemical reaction includes cavitating the liquid and/or inducing a shear force. The reactor should be one that can cause cavitation, shear, high pressure, high temperatures and/or mixing, such as a cavitation reactor, a shear reactor, or a mechanically agitated reactor. In some embodiments, the reactor is a mechanically agitated reactor containing a stirrer, where the stirrer induces a shear force in the liquid.

This document describes methods for producing a solid carbon material, where the method includes: delivering a liquid containing at least one liquid organic compound to a cavitation reactor; formation of cavitation bubbles in the liquid in the cavitation zone of the cavitation reactor; and delivering a gas containing at least one gaseous organic compound to the cavitation zone of the cavitation reactor; thus, obtaining a carbon material in the form of a dispersion containing a carbon material dispersed in a liquid. Optionally, the reactor is a hydrodynamic cavitation reactor, a shear reactor, an ultrasonic cavitation reactor, or a multifunctional reactor. Optionally, the cavitation reactor includes hydrodynamic cavitation or ultrasonic cavitation. Optionally, the reactor includes a rotor-stator reactor, shear stack reactor, high speed shear reactor (e.g. Charles Ross HSM-700), hydrodynamic cavitation reactor, sieve reactor, packed bed rotary reactor, rotary disk reactor, colliding jet reactor , supersonic gas-solid reactor, ultrasonic reactor, ultrasonic probe reactor, shear stirred reactor, microwave reactor, shock wave reactor (e.g. SHOCKWAVE POWER™ Reactor (SPR); Hydro Dynamics, Inc., Rome, GA), or a combination of them. In an embodiment, sonication is used to induce or induce cavitation in a liquid. Optionally, gas delivery includes gas capture, gas injection, or a combination thereof. Optionally, the gas is entrained in the liquid. The gas can be entrained in the liquid using any suitable pressure that allows gas-liquid mass transfer under reactor operating conditions (eg, 2-150 psi, 10-100 psi). Optionally, the gas is injected into the liquid. Optionally, the gas is bubbled into the liquid. Optionally, the gas is delivered directly to the cavitation zone during the gas delivery step. For example, the gas is delivered directly to the cavitation zone at the nucleation site of the cavitation bubbles. Optionally, the stages of cavitation bubble formation and gas delivery are performed simultaneously or almost simultaneously (for example, within 5 minutes, within 4 minutes, within 2 minutes, within 1 minute, within 30 seconds, within 15 seconds, within 10 seconds, within 5 seconds, or within 1 second). Optionally, during the gas delivery step, the gas is delivered directly to or within 1 mm of the cavitation bubble nucleation zone, where the cavitation bubble nucleation zone corresponds to the cavitation bubble nucleation in the hydrodynamic cavitation reaction during the formation step. Optionally, the formation step includes the formation of a cavitation cloud containing cavitation bubbles in the cavitation zone of the reactor, where the gas is delivered directly into or 1 mm from the cavitation cloud. Optionally, the dispersion is formed in the cavitation zone of the reactor. Optionally, the forming step includes forming a cavitation cloud containing cavitation bubbles; where the carbon material is formed in the cavitation cloud. Optionally, the liquid is substantially free of carbon material during the liquid delivery step and prior to the formation of cavitation bubbles. Optionally, the liquid is substantially free of solids and is essentially not a colloid, suspension, or sol during the liquid delivery step and prior to the formation of cavitation bubbles. Preferably, the preparation of the carbonaceous material comprises nucleating the carbonaceous material in a liquid. Preferably, the production of the carbon material includes nucleating the carbon material in the liquid and growing the carbon material in the liquid.

In one aspect, provided herein is a method for functionalizing a liquid-dispersed material, wherein the liquid-dispersed material is a first dispersion, wherein the method comprises the steps of: delivering the first dispersion to a cavitation reactor; where the liquid contains at least one liquid organic compound; formation of cavitation bubbles in the liquid in the cavitation zone of the hydrodynamic cavitation reactor; and delivering a gas containing at least one gaseous organic compound directly to the cavitation zone of the cavitation reactor; thus functionalizing the material to form a second dispersion, wherein the second dispersion contains the functionalized material dispersed in a liquid. In some embodiments, the functionalization of a material includes chemical, physical, or both chemical and physical functionalization of the material. In some embodiments, the material is a carbon material, including graphite, expanded graphite, graphite-like material, graphene, graphene-like material, carbon nanotubes, carbon onions, or other carbon allotrope, hexagonal boron nitride, or any combination thereof. In some embodiments, the functionalized material includes graphene oxide. In some embodiments, functionalization includes adding oxygen atoms to a material, removing oxygen atoms from a material, adding nitrogen atoms to a material, adding sulfur atoms to a material, or a combination thereof. In some embodiments, the gas includes oxygen, steam, hydrogen, nitrogen, sulfur dioxide, CO ₂ , ozone, or any combination thereof. In some embodiments, the gas is delivered directly to the cavitation zone during the gas delivery step. In some embodiments, the cavitation bubble formation and gas delivery steps are performed simultaneously or nearly simultaneously (e.g., within 5 minutes, within 4 minutes, within 2 minutes, within 1 minute, within 30 seconds, within 15 seconds, within 10 seconds, within 5 seconds, or within 1 second). In some embodiments, the step of forming the cavitation bubbles includes nucleating the cavitation bubbles. In some embodiments, during the gas delivery step, gas is delivered directly to or within 1 mm of the cavitation bubble nucleation zone, where the cavitation bubble nucleation zone corresponds to cavitation bubble nucleation in the hydrodynamic cavitation reaction during the formation step. In some embodiments, the formation step includes forming a cavitation cloud containing cavitation bubbles in the cavitation zone of the reactor, where the gas is delivered directly into or 1 mm from the cavitation cloud. In some embodiments, the material functionalization method includes terminating the gas delivery and keeping the dispersion in the cavitation zone while no gas is delivered to the cavitation zone. In some embodiments, during the stage of maintaining the dispersion in the cavitation zone and after the completion stage, and while no gas is delivered to the cavitation zone, the functionalization method further includes the step of degassing the dispersion to reduce the concentration of gas trapped therein.

BRIEF DESCRIPTION OF THE DRAWINGS

FIG. 1 illustrates a typical hydrodynamic cavitation reactor, or part thereof, in accordance with certain embodiments of the invention.

FIG. 2 shows a voltage versus current plot of untreated graphene, reduced graphene, and acetylene treated reduced graphene in an embodiment of the invention.

FIG. 3 shows a scanning electron microscopy (SEM) image of graphene-like plates obtained in accordance with an embodiment of the invention.

FIG. 4 shows a plot of energy (keV) versus intensity using X-ray energy dispersive spectroscopy (EDS) data measured on two portions of the plates shown in FIG. 3 (superposition of spectrum 5 and spectrum 6).

FIG. 5A and FIG. 5B show additional SEM images of exemplary graphene-like wafers obtained in embodiments of the methods described herein.

FIG. 6A-6B: FIG. 6A shows an SEM image of micron-sized graphene-like plates with squares (labeled "1" and "2") identifying regions corresponding to the EDS spectra shown in FIG. 6B (square 1 corresponds to "Spectrum 1" and square 2 corresponds to "Spectrum 2"). FIG. 6B shows the EDS spectra of the atomic concentrations of elements calculated from the EDS spectra in the carbon material in the regions defined in FIG. 6A.

FIG. 7A-7B: FIG. 7A shows an SEM image of micron-sized graphene-like plates with squares (labeled "5" and "6") identifying regions corresponding to the EDS spectra shown in FIG. 7B (square 5 corresponds to "Spectrum 5" and square 6 corresponds to "Spectrum 6"). FIG. 7B shows the EDS spectra and a table summarizing the atomic concentrations of elements calculated from the EDS spectra in the carbon material in the regions defined in FIG. 7A.

FIG. 8A-8B show SEM images of the carbon material according to Example 4B.

FIG. 9A-9B show light scattering intensity data for the carbon material according to Example 5A.

FIG. 10A-10B show the quantitative particle size distribution for the carbon material according to Example 5A.

FIG. 11A-11B show Zeta potential mobility data for the carbon material dispersion according to Example 5A.

FIG. 12A-12B show SEM images and EDS data corresponding to the carbon material of Example 5B.

FIG. 13A-13B show the SEM image and EDS data corresponding to the carbon material of Example 10.

FIG. 14 shows a Friction-to-Time plot for untreated Syn 530 engine oil (top) and processed Syn 530 engine oil (bottom), where "treated" refers to the method of producing the carbon materials described herein, according to certain embodiments. The data demonstrates that reduced wear marks and coefficient of friction from the presence of nanocrystalline carbon material formed during cavitation in Syn 530 engine oil incorporating captured propane gas using high shear, according to the embodiments described herein.

FIG. 15 shows a graph of Friction versus Time for untreated AMSOIL™ oil (top) and treated AMSOIL™ oil (bottom), where “treated” refers to the method of producing the carbon materials described herein, in accordance with certain embodiments. The data demonstrates reduced wear marks and coefficient of friction from the presence of nanocrystalline carbon material formed during cavitation in AMSOIL™ engine oil incorporating entrained propane gas using high shear, according to the embodiments described herein.

FIG. 16 shows a Friction-to-Time plot for untreated MOBILE 1™ oil (top) and treated MOBILE 1™ oil (bottom), where "treated" refers to the method of producing the carbon materials described herein, in accordance with certain embodiments. The data demonstrates reduced wear marks and coefficient of friction from the presence of nanocrystalline carbon material formed during cavitation in MOBILE 1™ engine oil incorporating entrained propane gas using high shear, according to the embodiments described herein.

FIG. 17A-17B show mobility data for determining the Zeta potential for the carbon material dispersion according to Example 11A.

FIG. 18 shows a schematic of a typical shift stack reactor.

FIG. 19 shows a diagram of a typical high speed shear reactor.

FIG. 20 shows a diagram of a typical multifunctional reactor.

FIG. 21 shows a diagram of a typical cavitation sonication reactor (eg, ultrasonic probe reactor).

FIG. 22 shows a plot of K _total to stirrer speed from the book, "Scaling Chemical Processes, Practical Guides in Chemical Engineering" by Jonathan Wostell, 2016.

FIG. 23 shows a typical mechanically agitated reactor, in accordance with certain embodiments.

FIG. 24 shows illustrations corresponding to a gas induction paddle for a mechanically stirred reactor.

FIG. 25 shows an SEM showing a low-layer graphene-like material produced in a high-temperature, high-pressure stirred reactor by injecting propane gas into liquid toluene for 30 minutes at 80 psi. and temperature 60°C.

FIG. 26 shows the EDS of atomic fractions of elements in graphene oxide.

FIG. 27 shows the EDS of element atomic fractions in reduced graphene oxide (reduced graphene oxide of FIG. 26).

FIG. 28 shows the EDS of the atomic fractions of elements in pure graphene.

FIG. 29 shows the EDS of atomic fractions of elements in partially oxidized (oxidized edge) graphene (oxidized graphene of FIG. 28).

FIG. 30 illustrates data showing that if water-dispersed oxidized edge graphene is added to the aqueous portion of Master Chemical 685, there is a 26% recovery in the torque required to form filaments in steel.

FIG. 31 shows Zeta potential data for cationic graphene prepared according to certain embodiments described herein.

STATEMENTS REGARDING CHEMICAL COMPOUNDS AND NOMENCLATURE

In general terms and phrases used herein have their usual meaning in the art as found by reference in standard texts, journal references, and from contexts known to those skilled in the art. The following definitions are provided to clarify their specific use in the context of the invention.

Without wishing to be bound by any particular theory, this document may be a discussion of the views or understanding of the basic principles regarding the devices and methods described in this document. It is recognized that regardless of the ultimate correctness of any mechanistic explanation or hypothesis, an embodiment of the invention may nevertheless be operable and useful.

As used herein, the term "organic compound" refers to a chemical species characterized by a chemical formula having at least one carbon atom (C). For example, methane (CH ₄ ) is a gaseous organic compound. For example, ethanol is a liquid organic compound. The term "liquid organic compound" refers to an organic compound that is essentially liquid under the conditions of the method in which it is used (for example, its boiling point is greater than the bulk temperature of the liquid during the process). The term "gaseous organic compound" refers to an organic compound that is essentially gaseous under the conditions of the process in which it is used (eg, its boiling point is less than the bulk temperature of the gas during the process being performed).

The term "cavitation" refers to the formation of vapor voids or "cavitation bubbles" in a liquid as a result of a change in pressure (usually a rapid pressure change) indicated by or transmitted to the liquid. For example, a fluid undergoing a sudden expansion, such as a fluid exiting a small orifice and entering a larger volume, may experience a sudden drop in pressure sufficient to cause cavitation bubbles to form. Cavitation can be caused by one or a combination of forces or energy sources, including, but not limited to, pressure change due to volume expansion, sonication (also referred to herein as sonication). Even though cavitation may occur in a high shear reactor, especially with gas injection, the main reaction is likely to occur as a result of shear. Hydrodynamic cavitation includes cavitation induced or caused by a change in pressure transmitted or experienced by a fluid, such as due to a change in volume, such as due to passage of the fluid into, through, and out of an orifice. Ultrasonic cavitation (also referred to herein as sonic cavitation or ultrasonic cavitation) refers to cavitation induced or caused by sonication transmitted to or by a liquid being tested. The formation of the cavitation bubble includes the first nucleation of the cavitation bubble. Cavitation can be associated with the formation of multiple cavitation bubbles, so that the sum of the cavitation bubbles existing at any given moment forms a "cavitation cloud". A cavitation cloud corresponds to a zone of fluid including cavitation bubbles, which, in some embodiments, includes any zone or location where a cavitation bubble nucleates.

As used herein, the term "cavitation reactor" refers to a reactor that induces or causes cavitation in a liquid. Preferably, but not necessarily, the cavitation reactor is a hydrodynamic cavitation reactor, an ultrasonic cavitation reactor, or a multifunctional cavitation reactor.

A "hydrodynamic cavitation reactor" is a reactor configured to induce or cause hydrodynamic cavitation in a liquid. Preferably, the hydrodynamic cavitation reactor is a system including one or more zones for inducing cavitation (formation of cavitation bubbles) in a liquid. A hydrodynamic cavitation reactor typically includes a pre-cavitation zone and a cavitation zone. In some embodiments, the hydrodynamic cavitation reactor includes at least one opening (eg, lumen, gap, channel, notch, perforation) such that fluid flows from the pre-cavitation zone, through the opening, into the cavitation zone. Hydrodynamic cavitation reactors used in the methods described herein may include a variety of configurations and zones/equipment for the formation of cavitation bubbles, including, but not limited to, holes, nozzles, venturis, rotors, and any combination thereof or other features known in this field of technology.

"Shear reactor", a reactor configured to induce or cause shear in a fluid. FIG. 18 shows that a typical shear stack reactor (shear reactor) such as the high shear FM Fuko Bench device. FIG. 19 shows a shear mixer such as the Charles Ross HSM-700 inline high speed rotor-stator type shear reactor which is also capable of inducing cavitation when gas is injected.

An "ultrasonic cavitation reactor" is a reactor configured to induce or cause ultrasonic cavitation in a liquid.

A "multifunctional reactor" is a reactor including a plurality of reactors or a plurality of different mechanisms/processes for inducing a chemical reaction through which a solid carbon material is produced. The multifunctional reactor may be a multifunctional cavitation reactor including a plurality of cavitation reactors, or a cavitation reactor inducing or causing cavitation in a liquid through a plurality of cavitation types (or energies or forces inducing or causing cavitation). For example, a multifunctional reactor may include a variety of mechanisms for inducing or inducing cavitation in a liquid. For example, a multifunctional reactor may be configured to induce or cause at least two of hydrodynamic cavitation, ultrasonic cavitation, and fluid shear. FIG. 20 shows a diagram of a multifunctional cavitation reactor including a hydrodynamic cavitation reactor and a shear reactor. According to certain embodiments, the multifunctional cavitation reactor includes two reactors connected in series as shown in FIG. 20. A first reactor, such as a hydrodynamic gas-fed cavitation reactor, can create solid carbon material, such as graphene-like materials, for example, by depressurizing the liquid as it passes through one or more orifices, and injecting gas near the nucleation point(s) of the cavitation bubble(s). In certain embodiments, the liquid (now filled with carbon material) is then passed through a second reactor, such as a high shear reactor, where the graphene-like material, for example, can be sheared into crystalline particles. According to certain embodiments, no gas is injected into the second reactor, such as a high shear reactor.

As used herein, the term "in situ" (or "in-situ") in relation to a solid carbon material or a process for producing a solid carbon material, such as an in situ formed carbon material or an in situ carbon material or an in situ process for producing a solid carbon material refers to a carbon material or a process for producing a solid carbon material, where the carbon material is obtained by said process and is not otherwise an input to the process. The process for producing the carbon material may be the method of any embodiment described herein, and the carbon material may be the carbon material(s) of any embodiment described herein. For example, the liquid introduced into the in situ process does not contain carbon material, and the solid carbon material is produced in the liquid during the in situ process, in which case the resulting carbon material may be referred to as in situ carbon material. For example, in an in situ process for producing a solid carbon material, the liquid is substantially free of carbon material during the liquid delivery step and prior to the formation of cavitation bubbles in said liquid during the in situ process. For example, the liquid is substantially free of solid particles and is essentially not a colloid, slurry, or sol during the stage of delivering the liquid to the process and prior to the formation of cavitation bubbles. As described elsewhere herein, in situ carbon material can be produced in a reaction zone of a reactor, such as a cavitation zone or cavitation cloud, of a cavitation reactor during a carbon material production process.

As used herein, the term "well-dispersed" may refer to particulate(s) in a liquid that are stably dispersed with little or no agglomeration and/or precipitation from the liquid. Preferably, but not necessarily, well-dispersed particles have a Zeta potential greater than +40 mV or less than -40 mV.

The term "dispersion" refers to a mixture of particles, such as particles of one or more solid carbon materials, dispersed and/or suspended in a liquid, which may be referred to as a solvent. The colloidal mixture is a typical dispersion. Preferably, but not necessarily, the dispersion is a homogeneous mixture. In the context of dispersion, the term "homogeneous" refers to a liquid mixture that appears homogeneous to the naked eye. Conversely, a heterogeneous liquid mixture includes particles that precipitate out of or are suspended in the liquid mixture and are large enough to be clearly identifiable to the naked eye in the liquid mixture. The heterogeneous liquid mixture includes, for example, settled and/or settling particles. Preferably, but not necessarily, the term "dispersion" is broadly intended to include solutions and dispersions, such as colloids, that are not heterogeneous liquid mixtures. Preferably, but not necessarily, the dispersion is a microscopically homogeneous or homogeneous mixture of particles in a liquid, such as a solvent. Preferably, but not necessarily, the dispersion is thermodynamically favorable to remain stably dispersed, or thermodynamically favorable to settling separation, but where settling is kinetically retarded or prevented. Particles, dispersions that are characterized as being stably dispersed, remain dispersed in the dispersion and do not precipitate or settle out of the dispersion liquid for at least 5 hours, preferably at least 12 hours, preferably at least 24 hours and more preferably at least 1 week, at normal temperature and pressure (NTP) and under the influence of air.

As used herein, the term "carbon material" refers to a solid carbon material. The term "carbon material" or "solid carbon material" as used herein does not refer to a liquid organic compound (such as a liquid organic compound of a fluid delivered to a reactor), and does not refer to a gaseous organic compound (such as a gaseous organic compound gas delivered to the reactor). Typical carbon materials include, but are not limited to, graphite, expanded graphite, graphite-like material, graphene, graphene-like material, carbon nanotubes, carbon onions, other carbon allotropes, graphene containing composite, cationic graphene, and any combinations thereof.

The term "simultaneous" refers to the same time within detection. The term "almost simultaneously" includes within 5 minutes, within 4 minutes, within 2 minutes, preferably within 1 minute, more preferably within 30 seconds, preferably within 15 seconds in some embodiments, preferably within in some embodiments, within 10 seconds, preferably, in some embodiments, within 5 seconds, or more preferably, in some embodiments, within 1 second.

A gas trapped in a liquid is, for example, a gas dissolved in a liquid. An injected gas is, for example, a gas injected, for example, through a pressure difference, into a liquid, such that the gas is injected into or otherwise exists in the liquid (eg, at the start of bubble formation). Bubbling a gas into a liquid is an example of injecting a gas into a liquid.

The term "bulk temperature" refers to the average temperature of a substantial fraction of a liquid or material. For example, the bulk temperature of the fluid may be about room temperature, even though the fluid may contain local variations in temperature, such as in situ cavitation bubble formation and collapse, where the local temperature may exceed the bulk temperature. For example, the local fluid temperature may correspond to the fluid temperature on a scale of 1 nm ³ or less, 10 μm ³ or less, 100 μm ³ or less, or 1 mm ³ or less. For example, the local temperature of the liquid may correspond to the temperature of the liquid on a scale greater than 1 mm ³ .

As used herein, the term "polymer" refers to a molecule composed of repeating structural units linked by covalent chemical bonds, often characterized by a significant number of repeating units (e.g., equal to or greater than 3 repeating units, optionally, in some embodiments, equal to or greater than 10 repeat units, in some embodiments, greater than or equal to 30 repeat units) and high number average molecular weight (e.g., greater than 1000 daltons, greater than or equal to 10,000 daltons, in some embodiments, greater than or equal to 50,000 Daltons or greater than or equal to 100,000 Daltons). Polymers are typically the polymerization product of one or more monomer precursors. The term polymer includes homopolymers, ie. polymers consisting essentially of a single repeating monomer subunit. The term polymer also includes copolymers formed when two or more different types of monomers are combined in one polymer. The copolymers can contain two or more monomer subunits and have random, block, brush, block-brush, alternating, segmented, graft, fusiform, and other architectures. Useful polymers include organic polymers or inorganic polymers, which may be in amorphous, semi-amorphous, crystalline or semi-crystalline states. Polymer side chains capable of cross-linking polymers (eg, physical cross-linking) may be useful in some areas. Useful copolymers include block copolymers and/or graft copolymers. Exemplary polymers include, but are not limited to, those having repeating units having one or more unsubstituted or substituted polyisocyanate groups, polymethacrylate groups, polyacrylate groups, polymethacrylamide groups, polyacrylamide groups, polyquinoxaline groups, polyguanidine groups, polysilane groups, polyacetylene groups, polyamino acid groups, polypeptide groups, polychloral groups, polylactide groups, polystyrene groups, polyacrylate groups, polytert- butyl acrylate groups, polymethyl methacrylate groups, polysiloxane groups, polydimethylsiloxane groups, poly-n-butyl acrylate groups, polyethylene glycol groups, polyethylene oxide groups, polyethylene groups, polypropylene groups, polytetrafluoroethylene groups, polyvinyl chloride groups, and any combination thereof.

As used herein, the term "group" refers to the functional group of a chemical compound. Compound data groups refer to the atom or collection of atoms that are part of the compound. The groups of the present invention may be attached to other atoms of the complex through one or more covalent bonds. Groups can also be characterized with respect to their valency. The present invention includes groups characterized by monovalent, divalent, trivalent, etc. valence.

"Oligomer" refers to a molecule composed of a repeat of structural units linked by covalent chemical bonds, often characterized by a number of repeat units less than that of a polymer (e.g., equal to or less than 3 repeat units) and a lower number average molecular weight (e.g., less than or equal to 1000 daltons) than polymers. The oligomers may be the polymerization product of one or more monomer precursors.

The term "prepolymer" or "prepolymer" refers to a monomer or a mixture comprising one or more monomers, where the monomer(s) react to an intermediate molecular weight state. The prepolymer is capable of further polymerization to a fully cured higher molecular weight state. In some embodiments, the terms prepolymer and monomer are used interchangeably.

Unless otherwise indicated, the term "molecular weight" refers to the average molecular weight. Unless otherwise indicated, the term "average molecular weight" refers to the number average molecular weight. The number average molecular weight is defined as the total volume weight of the sample divided by the number of molecules in the sample. As is commonly known in the art, peak average molecular weight and weight average molecular weight can also be used to characterize the molecular weight distribution of polymers in a sample.

The term "weight average molecular weight" (M _w ) refers to the average molecular weight, defined as the sum of the products of the molecular weight of each polymer molecule (M _i ) times its mass fraction ( _wi ): M _w =Σw _i M _i . As is commonly known in the art, peak average molecular weight and number average molecular weight can also be used to characterize the molecular weight distribution of polymers in a sample.

The term "substantially" refers to a property or condition that is 20%, 10%, 5%, 1%, or equivalent to a reference property or condition. The term "substantially equal", "substantially equivalent", or "substantially unchanged", when used in conjunction with a reference value describing a property or condition, refers to a property or condition that is 20%, 10%, 5%, 1%, 0.1%, or optionally equivalent to the reference value or condition provided. For example, the concentration is essentially equal to 1 wt. -%, if the concentration value is 20%, 10%, 5%, 1% or equal to 1% wt. For example, substantially all of a material or liquid is in a particular region if at least 80% (e.g., by volume, moles, or mass), at least 90%, at least 95%, at least 95 % or 100% of the material or liquid is in a particular area. The term "substantially greater" when used in conjunction with a reference value or condition describing a property or condition, refers to a value that is at least 2%, at least 5%, at least 10%, or , at least 20% greater than the presented reference value or condition. The term "substantially less" when used in conjunction with a reference value or condition describing a property or condition refers to a value or condition that is at least 2%, at least 5%, at least 10 % or at least 20% less than the reported reference value. For example, the concentration is substantially less than 1 wt % if the concentration value is at least 20% less than, at least 10% less than, at least 5% less than, or, at least 1% less than 1% of the mass.

The term "graphene-like material" refers to a solid carbon-based material obtained by the method of the invention, which can be processed to be physically akin to pure graphene. Pure graphene contains less than 1% oxygen and has few layers (eg 1-2 layers). The size of pure graphene plates, as a rule, varies from 1 to 5 microns. The in situ produced carbon material as described herein, and produced in a hydrocarbon solvent under hydrodynamic conditions, consists of multilayer lamellae (more than 2 layers, e.g. 5-15 layers, 6-13 layers, 7-12 layers, 8- 11 layers) with platelet sizes ranging from about 1 to 50 microns (eg, 2-25 microns, 3-15 microns, or 5-10 microns). When prepared with an anhydrous hydrocarbon solvent (eg, toluene), the resulting graphene-like material will have less than 1% oxygen. In addition, the graphene-like material obtained by the method of the invention is easily stratified in a liquid into several layers of graphene. It exfoliates more readily in a liquid than graphite because, without being bound by any theory, it is believed that since bulk graphene-like material is formed in situ, bulk graphene sheets can be held together by weaker van der Waals bonding than would be found in graphite.

The terms "stirred reactor" and "stirred reactor" are used interchangeably and have an equivalent meaning.

As used herein, the term "in situ friction reduction" refers to a process in which the lubricating properties of a fluid are altered or improved. In the process of reducing friction in situ, the fluid can be used as a lubricant and improve its lubricity at the same time or almost at the same time (for example, within 5 minutes, within 4 minutes, within 2 minutes, within 1 minute, within 30 seconds, within within 15 seconds, within 10 seconds, within 5 seconds, or within 1 second).

In an embodiment, a composition or compound of the invention, such as a liquid organic compound or a gaseous organic compound, is isolated or substantially purified. In an embodiment, the isolated or purified compound is at least partially isolated or substantially purified, as understood in the art. In an embodiment, a substantially purified composition, compound or formulation of the invention is chemically pure at least 95%, optionally at least 97% for some areas, optionally at least 98% for some areas, optionally, for some areas, at least 99%, optionally, for some areas, at least 99.9%, optionally, for some areas, 99.99%, and optionally, for some areas, 99.999%.

DETAILED DESCRIPTION OF THE INVENTION

In the following description, numerous specific details of the apparatuses, apparatus components, and methods of the present invention are set forth in order to provide a thorough explanation of the precise nature of the invention. Those skilled in the art, however, will appreciate that the invention may be practiced without these specific details.

The present document describes a method for producing a solid carbon material, including: delivering a liquid containing at least one liquid organic compound to a reaction zone of a reactor; delivering a gas containing at least one gaseous organic compound to the reaction zone of the reactor; and inducing a chemical reaction between at least one liquid organic compound and at least one gaseous organic compound, where: the chemical reaction occurs in the reaction zone of the reactor; solid carbon material obtained by the reaction; the solid carbon material is obtained during the reaction in the form of a dispersion comprising the solid carbon material dispersed in a liquid; and the chemical reaction is a homogeneous reaction involving homogeneous nucleation of solid carbon material in the reaction zone of the reactor. Preferably, the chemical reaction involves gas-liquid mass transfer. Preferably, but not necessarily, the composition of the gas is different from that of the liquid. Preferably, but not necessarily, the composition of the at least one gaseous compound is different from the composition of the at least one liquid organic compound. For example, the presence of a gas (or at least one gaseous organic compound) and a liquid (or at least one liquid organic compound) with a different chemical composition (for example, propane and ethanol) can provide a greater degree of flexibility in the type, composition and properties of the resulting solid carbon material(s), compared to an equivalent process where the gas and liquid have an equivalent chemical composition. Optionally, the chemical reaction does not occur on or with the catalyst. Preferably, but not necessarily, the method does not include heterogeneous nucleation of a solid carbon material on a solid support. Optionally, a liquid delivery step is performed via the first inlet stream to the reaction zone, and a gas delivery step is performed via the second inlet stream to the reaction zone; where the paths of the first stream and the second input stream are different and are physically separate. Optionally, the liquid delivery step and the gas delivery implementation step are performed simultaneously. Optionally, the gas delivery step is performed after the liquid is delivered to the reaction zone (for example, but not necessarily, by a batch process where the liquid is first delivered to the batch reactor and then the gas is delivered at a time when the reaction is desired). Preferably, the solid carbon material remains dispersed in the liquid while present in the reaction zone. Preferably, but not necessarily, the liquid is substantially free of solid carbon material during the liquid delivery stage and prior to the gas delivery and chemical reaction induction stages. Preferably, but not necessarily, the liquid is substantially free of solids and is substantially free of colloid, suspension, or sol during the liquid delivery step and up to the gas delivery and chemical reaction induction steps. Preferably, but not necessarily, the solid carbon material is formed only in the reaction zone of the reactor. Optionally, no solid carbon material is produced if the process is performed without a gas delivery step under otherwise equivalent steps and conditions. Preferably, but not necessarily, gas delivery includes gas capture, gas injection, or a combination thereof. Optionally, the gas is entrapped into the liquid under pressure, the gas is injected into the liquid, or the gas is bubbled into the liquid, or a combination thereof. Preferably, the gas is delivered directly to the reaction zone during the gas delivery step. The pressure in the reaction zone is any suitable pressure allowing gas-liquid mass transfer (eg, 10-5000 psi, 50-3000 psi, etc.). Preferably, but not necessarily, the gas delivery and chemical reaction induction steps are performed simultaneously or nearly simultaneously (e.g., within 5 minutes, within 4 minutes, within 2 minutes, within 1 minute, within 30 seconds, within 15 seconds , for 10 seconds, for 5 seconds, or for 1 second). Preferably, at least one liquid organic compound and at least one gaseous organic compound at the same time (for example, within 5 minutes, within 4 minutes, within 2 minutes, within 1 minute, within 30 seconds, within within 15 seconds, within 10 seconds, within 5 seconds, or within 1 second) are in the reaction zone. Preferably, the preparation of the carbonaceous material comprises nucleating the carbonaceous material in a liquid. Preferably, the production of the carbon material includes nucleation of the carbon material in the liquid and growth of the carbon material in the liquid. Optionally, the solid carbon material is a plurality of carbon materials. Optionally, the reactor is a cavitation reactor, a shift reactor, a mechanically stirred reactor, or a multifunctional reactor. In some embodiments, the reactor is a cavitation reactor; the reaction zone is the cavitation zone of the cavitation reactor; and the method includes forming cavitation bubbles in the liquid in the cavitation zone of the cavitation reactor.

Compared to conventional processes, the methods of the invention disclosed herein can take minutes or even seconds rather than hours, are low cost, minimally use unwanted chemicals, use less energy, and/or are highly scalable. Surprisingly, it has been found that according to the methods of the invention, a solid carbon material such as graphene or a graphene-like material can be obtained directly (ie, in one step) in a liquid in the form of a dispersion, including a stable dispersion. A dispersed solid carbon material (eg, graphene or a graphene-like material) has one or more advantages over a solid powder. These advantages include that liquids can be diluted much more easily than powder, liquids are easier to handle in terms of material handling, and/or producing solid carbon material directly, in one step, in a liquid is less expensive than making a powder and then powder dispersion.

In the method of the invention, the reactor is any suitable reactor that facilitates gas-liquid mass transfer to form a solid carbon material from at least one gaseous organic compound and at least one liquid organic compound. In general, the reactor will be one that can provide cavitation, shear, high pressure, high temperatures and/or mixing, or any combination of these conditions. In embodiments, the reactor is selected from the group consisting of a cavitation reactor, a shear reactor, a mechanically stirred reactor, or a combination thereof. Typical examples of a suitable reactor that can provide cavitation, shear, high pressure, high temperatures and/or mixing include mechanically stirred reactor, turbine reactor, monolithic reactor, foam reactor, rotor-stator reactor, shear stack reactor, high speed reactor shear (e.g. Charles Ross HSM-700), Hydrodynamic Cavitation Reactor, Sieve Reactor, Tubular Rotary Reactor, Packed Bed Rotary Reactor, Accordion Type Rotary Reactor, Fluidized Bed Reactor, Taylor-Couette Reactor, Double Tube Reactor, Rotary Disk Reactor , colliding jet reactor, ultrasonic gas-solid reactor, ultrasonic reactor, ultrasonic probe reactor, microwave reactor, shock wave reactor (e.g. SHOCKWAVE POWER™ Reactor (SPR); Hydro Dynamics, Inc., Rome, GA) , continuous flow reactor (e.g. RAPTOR™ reactor; La Mesta Chimie Fine, Gilette, France ), a shear stirred reactor, and any combination thereof. For example, a hydrodynamic cavitation reactor may be combined with a mechanically stirred reactor, or a mechanically stirred reactor may be combined with a shear reactor. It should be understood that the reactor can be classified into one or more categories for inducing gas-liquid mass transfer (eg, cavitation, shear, high pressure and/or high temperatures).

Optionally, the step of inducing a chemical reaction includes inducing a shear force in the fluid. Optionally, the reactor is a mechanically stirred reactor containing a stirrer; and where the agitator induces a shear force in the liquid. Optionally, the agitator is selected from the group consisting of a gas-inducing agitator, a Rushton/turbine agitator, a monolithic agitator, a helical agitator, a plate or radial flat agitator, axion propeller, angled blades, a turbine vortex agitator, multiple agitators on a single shaft, and any their combinations. Optionally, the stirrer is a gas-inducing stirrer. Optionally, the stirrer is characterized by a rotation speed selected from the range of 200 rpm to 14000 rpm (for example, 250-12000 rpm, 500-10000 rpm, 1000-5000 rpm, 1000-3000 rpm , 1000-1200 rpm). The shear created by the stirrer in a mechanically stirred reactor is mainly determined by the ratio of the impeller diameter (D) to the tank diameter (T). The D/T ratio is generally in the range 0.1-0.6, preferably 0.2-0.5. Low D/T ratios give high shear and typically spin at higher rpm, while high D/T ratios give low shear and spin at lower rpm. Optionally, the step of inducing a chemical reaction includes stirring or mixing the liquid and gas in the reaction zone, which may include reducing the average size of gas bubbles in the liquid in the reaction zone. Optionally, the pressure in the reactor zone is selected from the range of 6 bar (about 87 psi) to 150 bar (about 2175 psi). Optionally, the reaction zone temperature is selected from the range of 20°C to 250°C (e.g., 20°C to 200°C, 20°C to 150°C, 20°C to 100°C, 30° C to 250°C, 30°C to 200°C, 30°C to 150°C, 30°C to 100°C, 40°C to 250°C, 40°C to 200°C , 40°C to 150°C, 40°C to 100°C, 50°C to 250°C, 50°C to 200°C, 50°C to 150°C, 50°C up to 100°C, 50°C to 90°C or 60°C to 100°C).

In one aspect, provided herein is a method for producing a solid carbon material, wherein the method includes: delivering a liquid containing at least one liquid organic compound to a cavitation reactor; formation of cavitation bubbles in the liquid in the cavitation zone of the cavitation reactor; and delivering a gas containing at least one gaseous organic compound to the cavitation zone of the cavitation reactor; thus, obtaining a carbon material in the form of a dispersion, including a carbon material dispersed in a liquid. In some embodiments, the cavitation reactor is a hydrodynamic cavitation reactor, a shear reactor, an ultrasonic cavitation reactor, or a multifunctional reactor. In some embodiments, the cavitation reactor includes hydrodynamic cavitation; or the cavitation reactor includes ultrasonic cavitation. In some embodiments, the cavitation reactor includes hydrodynamic cavitation and a rotor-stator reactor; or the cavitation reactor includes ultrasonic cavitation and a rotor-stator type reactor. In some embodiments, the cavitation reactor includes a rotor-stator reactor, a battery shear reactor, a high speed shear reactor, a hydrodynamic cavitation reactor, a sieve reactor, a rotary packed bed reactor, a rotary disk reactor, a colliding jet reactor, an ultrasonic gas- a solid body, an ultrasonic reactor, an ultrasonic probe reactor, a shear stirred reactor, or a combination thereof. In some embodiments, gas delivery includes gas capture, gas injection, or a combination thereof. In some embodiments, the gas is entrapped in the liquid. In some embodiments, the gas is injected into the liquid. In some embodiments, the gas is bubbled into the liquid. In some embodiments, the gas is delivered directly to the cavitation zone during the gas delivery step. In some embodiments, the cavitation bubble formation and gas delivery steps are performed simultaneously or nearly simultaneously (e.g., within 5 minutes, within 4 minutes, within 2 minutes, within 1 minute, within 30 seconds, within 15 seconds, within 10 seconds, within 5 seconds, or within 1 second). In some embodiments, the step of forming cavitation bubbles includes nucleating cavitation bubbles. In some embodiments, during the gas delivery step, the gas is delivered directly to or within 1 mm of the cavitation bubble nucleation zone, where the cavitation bubble nucleation zone corresponds to the cavitation bubble nucleation in the cavitation reaction during the formation step. In some embodiments, the formation step includes forming a cavitation cloud including cavitation bubbles in the cavitation zone of the reactor, where the gas is delivered directly into or 1 mm from the cavitation cloud. In some embodiments, the dispersion is formed in the cavitation zone of the reactor. In some embodiments, the step of forming includes forming a cavitation cloud including cavitation bubbles; where the carbon material is formed in the cavitation cloud. In some embodiments, the liquid is substantially free of carbon material during the liquid delivery stage and prior to the formation of cavitation bubbles. In some embodiments, the liquid is substantially free of solids and is substantially free of colloid, suspension, or sol during the liquid delivery step and prior to the formation of cavitation bubbles. In some embodiments, obtaining the carbon material includes nucleating the carbon material in a liquid. In some embodiments, the production of carbon material includes the nucleation of the carbon material in the liquid and the growth of the carbon material in the liquid. In some embodiments, the carbon material is a plurality of carbon materials.

In some embodiments, the cavitation reactor is or includes a hydrodynamic cavitation reactor having a pre-cavitation zone and an orifice zone, where the orifice zone is between the pre-cavitational zone and the cavitation zone. The orifice zone includes at least one orifice such that liquid flows from the pre-cavitation zone to the cavitation zone through at least one orifice. In other words, during the liquid delivery step, liquid can be delivered to the pre-cavitation zone such that the liquid then flows out of the pre-cavitation zone, through at least one opening, into the cavitation zone. Each of at least one orifice has an internal diameter that is smaller than the internal diameter of the pre-cavitation zone. In some embodiments, the inner diameter of the cavitation zone immediately outside the at least one orifice is larger than the inner diameter of the orifice. In some embodiments, the gas is delivered directly to the cavitation end of at least one orifice or within 1 mm of the end of at least one orifice; where the cavitation end of at least one hole is the end of at least one hole closest to the cavitation zone of the cavitation reactor. In some embodiments, the gas is delivered at 1 mm (e.g., 0.8 mm, 0.6 mm, 0.5 mm, 0.3 mm, 0.2 mm) or directly to the outlet, at least at least one hole (for example, the end of one or more gas delivery pipes and gas is delivered there).

In some embodiments, during the gas delivery step, the gas is delivered directly to 1 mm, 0.8 mm, 0.6 mm, 0.5 mm, 0.3 mm, 0.2 mm, or 0.1 mm, or, preferably for some applications, directly into the nucleation zone of the cavitation bubble. The nucleation zone of the cavitation bubble corresponds to the nucleation site of the cavitation bubbles in the cavitation reaction during the formation stage. In some embodiments, during the gas delivery step, the gas is delivered directly to 1 mm, 0.8 mm, 0.6 mm, 0.5 mm, 0.3 mm, 0.2 mm, or 0.1 mm, or, preferably for some applications, directly into the reaction zone (eg, cavitation zone) of the reactor.

In some embodiments, the formation step includes the formation of a cavitation cloud including cavitation bubbles in the cavitation zone of the reactor, where the gas is delivered directly to 1 mm, 0.8 mm, 0.6 mm, 0.5 mm, 0.3 mm or 0.2 mm, or, preferably for some areas, directly into the cavitation cloud.

In some embodiments, the dispersion is at least partially formed in the reaction zone (eg, cavitation zone) of the reactor. In some embodiments, the dispersion is substantially formed in the reaction zone (eg, cavitation zone) of the reactor. In some embodiments, the dispersion is at least partially formed in the cavitation cloud of the reactor (if the reactor is a cavitation reactor). In some embodiments, the dispersion is substantially formed in the cavitation cloud of the reactor (if the reactor is a cavitation reactor). In some embodiments, the dispersion is at least partially formed in the nucleation zone of the cavitation bubble of the reactor (if the reactor is a cavitation reactor).

In some embodiments, the step of forming includes forming a cavitation cloud including cavitation bubbles; where the carbon material is formed in the cavitation cloud. In some embodiments, the liquid is substantially free of carbon material or crystals thereof during the liquid delivery step and prior to the formation of cavitation bubbles. For example, the liquid is substantially free of carbon material or crystals thereof prior to delivery of the liquid. In some embodiments, the liquid is substantially free of carbon material or crystals thereof prior to the liquid entering the cavitation zone of the cavitation reactor. For example, the liquid is substantially free of carbon material or crystals thereof until the liquid enters the orifice area of the hydrodynamic cavitation reactor. For example, the liquid is substantially free of carbon material or crystals thereof until the liquid exits the orifice of the orifice zone of the hydrodynamic cavitation reactor. For example, the liquid is essentially free of carbon material or its crystals until the liquid enters the interior, 1 mm, or 1 cm from the area of nucleation of cavitation bubbles. In some embodiments, the liquid is substantially free of solids and is essentially not a colloid, suspension, or sol during the liquid delivery step and prior to the formation of cavitation bubbles. For example, the liquid is substantially free of solid particles and is essentially not a colloid, slurry, or sol until the liquid enters the orifice of the orifice zone of the hydrodynamic cavitation reactor. In some aspects, the liquid is substantially free of solid particles and is essentially not a colloid, slurry, or sol prior to exiting the liquid from the orifice of the orifice zone of the hydrodynamic cavitation reactor. For example, the liquid is substantially free of solid particles and is essentially not a colloid, suspension, or sol until the liquid enters within 1 mm, or 1 cm, of the cavitation bubble nucleation region.

In some embodiments, the formation or nucleation of the carbon material occurs within 1 minute (eg, within 30 seconds, 20 seconds, 5 seconds, or 1 second) after the formation of cavitation bubbles in the liquid. In some embodiments, nucleation of the carbon material occurs within 1 minute (e.g., 30 seconds, 20 seconds, 5 seconds, or 1 second) after nucleation of 1 mm cavitation bubbles (e.g., 0.8 mm, 0.6 mm , 0.5 mm, 0.3 mm or 0.2 mm) of the nucleation zone of cavitation bubbles, while the gas is delivered to the cavitation zone.

In some embodiments, the method for producing a solid carbon material includes the step of completing the delivery of gas to a reaction zone (eg, a cavitation zone). The dimensional characteristics of the carbon material may change, decrease, or, preferably in some areas, increase after the completion stage. For example, particles of carbon material such as graphene particles or crystals thereof can increase in: the number of graphene layers, the length of the particle or layer, the width of the particle or layer, the diameter of the particle or layer, the thickness of the particle or layer, or any combination thereof. For example, carbon material particles such as graphene particles or crystals thereof can shrink in: the number of graphene layers, particle or layer length, particle or layer width, particle or layer diameter, particle or layer thickness, or any combination thereof. For example, back pressure (for example, through closing a valve below the cavitation zone and the liquid remaining there while continuing to deliver liquid) and/or edge shear (for example, for liquid flowing through an orifice) can lead to a decrease in the dimensional characteristics of the carbon material, for example, a decrease in the size graphene plates or the number of layers in graphene plates. In some embodiments, the process for producing a solid carbon material includes holding the dispersion in a reaction zone (e.g., cavitation zone) for a time that is less than or equal to 60 minutes (e.g., less than or equal to 30 minutes, less than or equal to 20 minutes, less than or equal to 10 minutes, less than or equal to 5 minutes, less than or equal to 1 minute) or selected from the range of 1-60 minutes, 2-60 minutes, 1-30 minutes, 1-20 minutes, 1-10 minutes, or, preferably for some areas, 1-5 minutes after the completion stage and in the absence of gas delivery to the reaction zone (eg, cavitation zone). For example, the dispersion (or liquid containing dispersed carbonaceous material) may circulate or otherwise remain at least partially or substantially in the reaction zone (eg, cavitation zone) after gas delivery is completed or otherwise disabled. For example, the valve may be at least partially closed below the reaction zone (eg, cavitation zone) during the storage stage to at least partially retain the dispersion in the reaction zone (eg, cavitation zone). For example, while maintaining the dispersion in the cavitation zone, the dispersion is at least partially or essentially in the cavitation cloud for at least 1%, at least 10%, at least 20%, at least at least 50% or at least 75% of the duration of the storage stage. For example, while maintaining the dispersion in the cavitation zone, the dispersion may be at least partially or essentially in the nucleation zone of the cavitation bubble for at least 1%, at least 10%, at least 20% , at least 50% or at least 75% of the duration of the storage stage. In some embodiments, during the storage step, the dimensional property of the carbon material may change, decrease, or, preferably in some areas, increase. In some embodiments, the concentration of carbon material in the dispersion remains substantially constant during the storage step after gas delivery is completed and in the absence of gas delivery to the reaction zone (eg, cavitation zone). In some embodiments, the concentration of carbonaceous material in the dispersion decreases during the storage step after gas delivery is completed. For example, the carbon material may nucleate in liquid during the gas delivery step, but the carbon material may substantially cease nucleating after the gas delivery is completed, although one or more of the carbon material's dimensional characteristics may continue to change. For example, due to the cessation of the nucleation of the carbon material, the concentration of the carbon material may be constant or may decrease if, for example, the particles of the carbon material stick together (e.g., aggregate and/or agglomerate) and/or the volume of the liquid corresponding to the dispersion increases. In some embodiments, during the step of maintaining the dispersion in the reaction zone (e.g., cavitation zone) and after the completion step and in the absence of gas delivery to the reaction zone (e.g., cavitation zone), the method of creating a solid carbon material further comprises the step of degassing the liquid or dispersion to reduce the concentration of gas trapped in it.

In some embodiments, a method for creating a solid carbon material includes restoring the carbon material from a dispersion, in solid or powder form. The recovery step may include, for example, filtration, vacuum filtration, solvent evaporation, centrifugation, or any combination thereof.

In some embodiments, the concentration of at least one liquid organic compound in the liquid (eg, water) is selected from the range of 1% wt. up to 100% wt. In an embodiment, the concentration of at least one liquid organic compound in the liquid is selected from a range of 25 wt. to 100% wt.

In some embodiments, the concentration of the resulting solid carbon material in the liquid is selected from the range of about 0.0025 wt%. up to 7% wt. (for example, from 0.0075% wt. to 7% wt., from 0.01% wt. to 5% wt., from 0.1% wt. to 5% wt., from 0.5% wt. to 4% wt., 1% wt. to 3% wt., 1% wt. to 2% wt.). The desired concentration may depend on the end use of the carbon material dispersion. For example, for a lubricating fluid, the desired concentration may be essentially about 0.01% of the mass. carbon material. For example, in order to obtain graphene powder, the concentration may be essentially about 5% of the mass. carbon material.

In some embodiments, at least one liquid organic compound comprises or is selected from the group consisting of a monomer, an oligomer, a prepolymer, a polymer, an organic solvent, and any combination thereof. In some embodiments, the implementation of at least one liquid organic compound includes thermoplastic polyurethane TPU and/or epoxy. In some embodiments, at least one liquid organic compound comprises or is selected from the group consisting of methanol, ethanol, isopropyl alcohol, methylpyrrolidone, d-cyclopentadiene, hexane, benzene, toluene, heptane, xylene, dimethyl sulfoxide, mineral oil, machine oil oil, MOBILE 1™ machine oil, Syn 530 machine oil, AMSOIL™, NonSyn, QUAKER STATE™ 530, base oil, hydrogenated castor oil, gear oil, gear oil, vegetable oil, hydrocarbon based drilling fluid, oils with additives, oils without additives (e.g. high carbon oil), kerosene, diesel fuel, ethylene glycol, propylene glycol, diethylene glycol, triethylamine, trimethylamine, pentane, cyclopentane, cyclohexane, 1,4-dioxane, chloroform, diethyl ether, dichloromethane, tetrahydrofuran, ethyl acetate, acetone, dimethylformamide, acetonitrile, nitromethane, propylene carbonate, formic acid, butanol, propanol, vinegar acid, octadecene, oleic acid, oleylamine, octane, diethylene glycol ether, 1,2-dichlorobenzene, methyl acetate, tetrachlorethylene, diphenylthiourea, hexafluoro-2-propanol, cinnamic acid, trimethylamine, benzenethiol, ethanethiol, ethanedithiol, 4-aminobenzenethiol, acrylic acid , carbon disulfide, 1,2-dichlorobenzene, N-methyl-2-pyrrolidone, and any combination thereof.

In some embodiments, the gaseous organic compound comprises or is selected from the group consisting of alkane, alkene, alkyne, cycloalkane, heterocycloalkane, arene, heteroarene, and combinations thereof. The alkane may be, for example, C _1-20 alkanes, C _1-12 alkanes, C _1-8 alkanes, C _1-6 alkanes, C _1-4 alkanes. The alkene may be, for example, C _1-20 alkenes, C _1-12 alkenes, C _1-8 alkenes, C _1-6 alkenes, C _1-4 alkenes. The alkyne may be, for example, C _1-20 alkynes, C _1-12 alkynes, C _1-8 alkynes, C _1-6 alkynes, C _1-4 alkynes. The cycloalkane may be, for example, C _3-10 cycloalkane, C _3-6 cycloalkane. The heterocycloalkane may be, for example, a stable, saturated or partially unsaturated monocyclic, bicyclic and spiro ring system containing 3-7 ring carbon atoms and other heteroatoms selected from N, S, and/or O. Examples of such heterocycloalkanes include isoxazole, thiazoline, imidazolidine, piperazine, homopiperazine, pyrrole, pyrroline, pyrazole, pyran, piperidine, oxazole and morpholine. The arene may be, for example, C _6-30 arenes, C _6-18 arenes, C _6-10 arenes, such as benzene and naphthalene. The heteroarene may be, for example, an aromatic 5- or 6-membered monocyclic group, a 9- or 10-membered bicyclic group, or an 11-14-membered tricyclic group, each containing at least one heteroatom (O, S, or N) in at least one of the rings, and each ring has at least one carbon atom. Illustrative examples of heteroarene include pyridine, pyridazine, pyrimidine, pyrazine, benzimidazole, triazine, imidazole, (1,2,3)- and (1,2,4)-triazole, pyrazine, tetrazole, furan, benzofuran, pyrrole, thiene, isothiazole , thiazole, isoxazole and oxadiazole). Alkane, alkene, alkyne, cycloalkane, heterocycloalkane, arene and heteroarene may be optionally substituted with one or more substituents (e.g. 1-5, 1-4, 1-3 or 1 or 2) such as alkyl, aryl, halogen (F , Cl, Br, I), nitro ((-NO ₂ ), cyano (-CN), hydroxy (-OH), thiol (-SH), alkoxy (-OR), formyl (-C (O) H), carboxy (-COOH), carboxyalkyl (-RCOOH), alkylcarboxy (-C(O)OR), amido (-C(O)NH or -NHC(O)H), mono- or dialkylamido (-C(O)NRR ´ or -NRC(O)H), amino or mono- or dialkylamino, where R is alkyl and R´ is hydrogen or alkyl, as described herein.

Examples of the gaseous organic compound include methane, acetylene, ethylene, propane, 1,3-butadiene, butane, and any combination thereof.

The gaseous organic compound is delivered at a flow rate suitable for the type of reactor and conditions used. In some embodiments, the gaseous organic compound has a flow rate selected from the range of 6 ml/min to 15 ml/min (e.g., 6 ml/min to 12 ml/min, 7 ml/min to 10 ml/min) in the reaction zone of the reactor, especially when the reactor is a hydrodynamic cavitation reactor, a shear stack reactor, or a high speed shear reactor (eg Charles Ross HSM-700).

In some embodiments, the gas contains a reducing compound (eg, hydrogen), an oxidizing compound (eg, oxygen, ozone, peroxide, or water), an inert compound (eg, argon, nitrogen), or any combination thereof.

In some embodiments, the liquid has a bulk temperature of less than 400°C, less than 300°C, less than 200°C, less than or equal to 100°C, less than or equal to 80°C, less than or equal to 50°C, less than or equal to 40°C, less than or equal to 35°C and/or 20°C or more in the reaction zone (eg, cavitation zone). In some embodiments, the gas has a bulk temperature of less than 400°C, less than 300°C, less than 200°C, less than or equal to 100°C, less than or equal to 80°C, less than or equal to 50°C, less than or equal to 40°C, less than or equal to 35°C and/or 20°C or more in the reactor, optionally in or near the reaction zone (eg, cavitation zone). Any two of the preceding endpoints may be used to define a closed range, or a single endpoint may be used to define an open range.

In some embodiments, the fluid has a flow rate selected from the range of 5 L/min to 200 L/min (e.g., 5 L/min to 100 L/min, 5 L/min to 50 L/min, 10 L/min /min to 200 l/min or 10 l/min to 100 l/min) in the reaction zone of the reactor, such as the cavitation zone of a hydrodynamic cavitation reactor or a sonication cavitation reactor, a shear reactor or a mechanically stirred reactor. In some embodiments, the gas is delivered (eg, injected) at a pressure selected from a range of 2 psi to 2 psi. up to 150 psi (e.g. 2-100 psi, 5-100 psi, 10-90 psi, 20-70 psi) in the reaction zone (for example, the cavitation zone). In some embodiments, the reaction zone pressure (eg, cavitation zone) is selected from the range of 10 psi to 10 psi. up to 5000 psi (e.g. 200 psi to 4000 psi, 1000-3000 psi). In some embodiments, the reactor includes a rotor-stator, and the rotor-stator operates at a rotation speed selected from a range of 200 rpm to 14,000 rpm (e.g., 250-12,000 rpm, 500-10,000 rpm, 1000-5000 rpm, 1000-1200 rpm) in the reaction zone (eg cavitation zone) of the reactor. In some embodiments, the residence time of the liquid in the reactor (eg, cavitation reactor) is selected from the range of 0.05 to 20 seconds. In some embodiments, the method is performed for a process time of at least 1 minute and preferably up to 60 minutes (e.g., at least 2 minutes, at least 5 minutes, at least 10 minutes and/ or up to 15 minutes, up to 20 minutes, up to 30 minutes, up to 40 minutes, up to 50). Any two of the above endpoints can be used to define a closed range, or a single endpoint can be used to define an open range. In some embodiments, the reactor (eg, cavitation reactor) includes an ultrasonic reactor, where the ultrasonic reactor is operated at a sonication frequency of 20 kHz to 300 kHz and an amplitude range of 10-100%.

In general, no solid carbon material is produced when the process is carried out in the absence of a gas delivery step under otherwise equivalent steps and conditions.

In some embodiments, the method for making a hard carbon material includes functionalizing the hard carbon material to produce a functionalized hard carbon material. In some embodiments of the method for producing a solid carbon material, the dispersion is the first dispersion, the carbon material is the precursor material, and the cavitation reactor is the first cavitation reactor; the method further includes: delivering the first dispersion to the second cavitation reactor; formation of cavitation bubbles in the first dispersion in the cavitation zone of the second cavitation reactor; and delivering the gas, including at least one gaseous organic compound, directly to the cavitation zone of the second cavitation reactor; thereby converting the precursor material into a second carbon material, wherein the second carbon material, in the form of a second dispersion, comprises the second carbon material dispersed in the liquid; where the precursor material and the second carbon material are different. In some embodiments, the first cavitation reactor and the second cavitation reactor are the same.

In some embodiments, the dispersion is the first dispersion, the chemical reaction is the first chemical reaction, the gas is the first gas, the reactor is the first reactor, and the solid carbon material is the precursor material. In such embodiments, the method further comprises: delivering the first dispersion to the second reactor; delivering a second gas containing at least one gaseous organic compound directly to the reaction zone of the second reactor; and inducing a second chemical reaction in the reaction zone of the second reactor; where: the second chemical reaction converts the precursor material into a second solid carbon material; where the second carbon material is dispersed in the liquid; and the precursor material and the second carbon material are different. Optionally, the second reactor is a cavitation reactor and the induction step includes forming cavitation bubbles in the first dispersion in the reaction zone of the second reactor, as described herein. Optionally, the first reactor and the second reactor are the same.

In some embodiments, the dispersion is a colloid, a suspension, or a combination thereof. In some embodiments, the carbon material comprises graphite , expanded graphite, graphite-like material, graphene, graphene-like material, carbon slabs, carbon nanotubes, carbon onions, another carbon allotrope, graphene-containing composite, cationic graphene, or any combination thereof. In some embodiments, the carbon material contains sulfur and graphene, or contains hexagonal boron nitride and graphene. In some embodiments, the carbon material comprises graphene or a graphene-like material. In some embodiments, the carbon material is graphene or a graphene-like material. In some embodiments, the carbon material comprises a graphene polymer nanocomposite. In some embodiments, the graphene is wrinkled graphene, crushed graphene, holed graphene, or any combination thereof.

In some embodiments, the solid carbon material has an oxygen content of less than or equal to 10% atom. (e.g. less than or equal to 7% atom, less than or equal to 5% atom, less than or equal to 1% atom, less than or equal to 0.5% atom, or less than or equal to 0.1% atom.) ("% atom." is an atomic percentage). In some embodiments, the carbon material has a carbon:oxygen atomic concentration ratio such as at least 150:1, at least 175:1, at least 200:1, at least 225:1, or at least 249:1. In some embodiments, the carbon material is substantially free of oxygen. In some embodiments, the carbon material is crystalline (eg, crystalline graphene). In some embodiments, hydrodynamic cavitation creates micron graphene-like plates. In some embodiments, the high shear results in a crystalline graphene material. In some embodiments, the dispersion or carbon material in the dispersion has a Zeta potential greater than +40 mV or less than -160 mV. In some embodiments, the dispersion or carbon material in the dispersion has a Zeta potential greater than +20 mV or less than -20 mV. In some embodiments, the dispersion or carbon material in the dispersion has a Zeta potential greater than +30 mV or less than -30 mV. In some embodiments, the dispersion or carbon material in the dispersion has a Zeta potential greater than +40 mV or less than -40 mV. In some embodiments, the dispersion or carbon material in the dispersion has a Zeta potential greater than +50 mV or less than -50 mV. In some embodiments, the dispersion or carbon material in the dispersion has a Zeta potential greater than +60 mV or less than -60 mV. In some embodiments, the dispersion or carbon material in the dispersion has an absolute Zeta potential value selected from the range of 20 mV to 100 mV. In some embodiments, the dispersion or carbon material in the dispersion has an absolute Zeta potential value selected from the range of 20 mV to 80 mV. In some embodiments, the dispersion or carbon material in the dispersion has an absolute Zeta potential value selected from the range of 20 mV to 70 mV. In some embodiments, the dispersion or carbon material in the dispersion has an absolute Zeta potential value selected from the range of 20 mV to 60 mV. In some embodiments, the dispersion or carbon material in the dispersion has an absolute Zeta potential value selected from the range of 20 mV to 50 mV. In some embodiments, the dispersion has a coefficient of friction that decreases by at least 5%, preferably by at least 10%, more preferably by at least 20%, even more preferably by at least 30% and further more preferably at least 50% relative to the same liquid without solid carbon material.

It has been found that in situ formation of a solid carbon material in the dispersion increases fluid lubrication. The improvement can be measured in terms of wear track recovery and/or coefficient of friction to the same fluid without the hard carbon material. In some embodiments, the dispersion has a wear track reduced by at least 3%, optionally at least 5%, preferably at least 10%, more preferably at least 20% , even more preferably at least 30% and further more preferably at least 50% relative to the same liquid without solid carbon material. The wear mark value can be measured by any suitable technique, including ASTM D 4172, Four Ball Wear Oil with Friction Coefficient Plot. In some embodiments, the method further comprises using a hard carbon material or dispersion to reduce friction. In some embodiments, the dispersion reduces the coefficient of friction by at least 5% (e.g., at least 10%, at least 20%, at least 30%, at least 40 %, at least 50% and/or up to 80%, up to 70%, up to 60% or up to 50%). Any two of the preceding endpoints may be used to define a closed range, or a single endpoint may be used to define an open range. In some embodiments, the dispersion is used to reduce friction without scrubbing or isolating the carbon material from the dispersion. In some embodiments, the carbon material or dispersion is a part of the battery (eg, a battery anode and/or a battery cathode), a conductive material, a heat transfer material, a lubricating fluid, and/or a heat transfer fluid. Optionally, the method includes in situ friction reduction.

In some embodiments, the reactor (eg, cavitation reactor, mechanically stirred reactor) includes a cooling system. In some embodiments, the reactor (eg, cavitation reactor, mechanically stirred reactor) comprises a heat exchanger and/or a cooler. In some embodiments, the reactor (eg, cavitation reactor, mechanically stirred reactor) contains a plurality of reaction zones (eg, cavitation zones). In some embodiments, the hydrodynamic cavitation reactor includes a plurality of holes.

Also described herein is a method for functionalizing a first solid carbon material dispersed in a liquid, wherein the first solid carbon material precursor is dispersed in a liquid that is the first dispersion, where the method includes the steps of: delivering the first dispersion to a reactor reaction zone; where the liquid contains at least one liquid organic compound; delivery of gas to the reaction zone of the reactor; and inducing a functionalization chemical reaction, wherein: the functionalization chemical reaction forms a second carbon material from the first carbon material; the functionalization chemical reaction takes place in the reaction zone of the reactor; and the second solid carbon material is obtained during the reaction in the form of a second dispersion, where the second dispersion includes a second solid carbon material dispersed in a liquid. Optionally, the functionalization chemistry includes chemical, physical, or both chemical and physical functionalization of the first solid carbon material. Optionally, the first solid carbon material comprises graphene oxide, graphite , expanded graphite, graphite-like material, graphene, graphene-like material, carbon slabs, carbon nanotubes, carbon onions, another carbon allotrope, graphene-containing composite, cationic graphene, or any combination thereof. Optionally, the second solid carbon material comprises, reduced graphene oxide, graphene oxide, edge-oxidized graphene, graphite , expanded graphite, graphite-like material, graphene, graphene-like material, carbon slabs, carbon nanotubes, carbon onions, another carbon allotrope, graphene containing composite , cationic graphene, or any combination thereof. Optionally, the first hard carbon material contains graphene oxide and the second hard carbon material contains reduced graphene oxide. Optionally, the atomic fraction of oxygen in the second carbon material is at least 50% less than the atomic fraction of oxygen in the first carbon material. Optionally, the functionalization chemistry includes oxidizing the first solid carbon material such that the second solid carbon material is soluble in water. Optionally, the liquid includes water and the second dispersion is an aqueous dispersion of the second carbon material in water. Optionally, the functionalization chemistry includes adding oxygen atoms to the first solid carbon material, removing oxygen atoms from the first solid carbon material, adding carbon atoms to the first solid carbon material, adding nitrogen atoms to the first solid carbon material, adding sulfur atoms to the first solid carbon material or a combination of them. Optionally, the gas contains oxygen, water vapor, hydrogen, nitrogen, sulfur dioxide, CO ₂ , ozone, or any combination thereof. Optionally, the reactor is a cavitation reactor and the reaction zone is a cavitation zone; the method includes the formation of cavitation bubbles in the liquid in the cavitation zone of the cavitation reactor; and the gas is injected directly into the cavitation zone. Optionally, the first solid carbon material is not chemically bonded to the solid support during the functionalization chemical reaction. Optionally, the gas contains at least one gaseous organic compound (eg, methane, acetylene, ethylene, propane, 1,3-butadiene, butane, and combinations thereof).

In one aspect, provided herein is a method for functionalizing a liquid-dispersed material, wherein the liquid-dispersed material is a first dispersion, the method comprising the steps of: delivering the first dispersion to a cavitation reactor; where the liquid contains at least one liquid organic compound; formation of cavitation bubbles in the liquid in the cavitation zone of the hydrodynamic cavitation reactor; and delivering a gas containing at least one gaseous organic compound directly to the cavitation zone of the cavitation reactor; thus functionalizing the material to form a second dispersion, wherein the second dispersion comprises a functionalized material dispersed in a liquid. In some embodiments, the functionalization of a material includes chemical, physical, or both chemical and physical functionalization of the material. In some embodiments, the material comprises graphene, carbon nanotubes, carbon onions, another carbon allotrope, hexagonal boron nitride, or any combination thereof. In some embodiments, the functionalized material contains graphene oxide. In some embodiments, functionalization includes adding oxygen atoms to a material, removing oxygen atoms from a material, adding nitrogen atoms to a material, adding sulfur atoms to a material, or a combination thereof. In some embodiments, the gas contains oxygen, steam, hydrogen, nitrogen, sulfur dioxide, or any combination thereof. In some embodiments, the gas is delivered directly to the cavitation zone during the gas delivery step. In some embodiments, the cavitation bubble formation and gas delivery steps are performed simultaneously or nearly simultaneously (eg, within 5 minutes, within 4 minutes, within 2 minutes, within 1 minute, within 30 seconds). In some embodiments, the step of forming the cavitation bubbles includes nucleating the cavitation bubbles. In some embodiments, during the gas delivery step, gas is delivered directly to or within 1 mm of the cavitation bubble nucleation region, where the cavitation bubble nucleation region corresponds to cavitation bubble nucleation in the cavitation reaction during the formation step. In some embodiments, the formation step includes forming a cavitation cloud including cavitation bubbles in the cavitation zone of the reactor where the gas is delivered directly within or within 1 mm of the cavitation cloud. In some embodiments, the method of functionalizing the material includes completing gas delivery and maintaining the dispersion in the cavitation zone, while not delivering gas to the cavitation zone. In some embodiments, during the stage of maintaining the dispersion in the cavitation zone and after the completion stage and in the absence of gas delivery to the cavitation zone, the functionalization method further includes the step of degassing the dispersion to reduce the concentration of gas trapped therein.

In some embodiments, the hydrodynamic cavitation reactor includes a pre-cavitation zone and an orifice zone, where the orifice zone is between the pre-cavitation zone and the cavitation zone. The orifice zone includes at least one orifice such that liquid flows from the pre-cavitation zone to the cavitation zone through at least one orifice. In other words, during the liquid delivery step, liquid can be delivered to the pre-cavitation zone such that liquid subsequently flows out of the pre-cavitation zone through at least one opening into the cavitation zone. Each of at least one of the holes is characterized by an inner diameter of the hole, which is less than the inner diameter of the pre-cavitation zone. In some embodiments, the internal diameter of the cavitation zone immediately outside the at least one orifice is greater than the internal diameter of the orifice. In some embodiments, gas is delivered at 1 mm (e.g., 0.8 mm, 0.6 mm, 0.5 mm, 0.3 mm, 0.2 mm) or directly to the end (e.g., exit) of at least one opening (for example, the end of one or more pipes for degassing and delivering gas there).

Also described herein is a process for producing a solid carbon material or a dispersion thereof, comprising any one or any combination of embodiments of the methods described herein, including methods for producing a solid carbon material and methods for functionalizing a material. Also described herein is a method for functionalizing a hard carbon material, including any one or any combination of embodiments of the methods described herein, including methods for producing a hard carbon material and methods for functionalizing a material.

Included herein are methods for producing solid carbon materials that are compatible with a variety of reactor technologies. Generally, and without wishing to be bound by any particular theory, the reactors used in the processes described herein facilitate a chemical reaction involving gas-liquid mass transfer to produce solid carbon material(s). Reactors facilitating a chemical reaction involving gas-liquid mass transfer to produce solid carbon material(s) will be referred to herein as "gas-liquid mass transfer reactors". Cavitation reactors, such as those described herein, may be typical gas-liquid mass transfer reactors that facilitate a chemical reaction that include gas-liquid mass transfer to produce solid carbon material(s). Shift reactors, such as those described herein, may be typical gas-liquid mass transfer reactors facilitating a chemical reaction involving gas-liquid mass transfer to produce solid carbon material(s). In certain embodiments, mechanically agitated reactors such as those described herein, including agitators such as a gas-inducing agitator, can provide shear to facilitate a chemical reaction involving gas-liquid mass transfer to produce solid carbon material(s). Suitable reactors that can be used as gas-liquid mass transfer reactors according to the embodiments described herein include, but are not limited to: stirred or spinning reactors (including turbine, monolithic, and foam reactors), tubular spinning reactors (including packed-bed, bellows, fluidized-bed, Taylor-Couette and twin-tube), rotating disk reactors (including rotor-stator, thin film and rotating disk reactors), shock wave and continuous flow reactors.

It should be noted, however, that the reactors described herein, such as cavitation reactors and mechanically stirred reactors, for example, are not necessarily gas-liquid mass transfer reactors or are not necessarily (inherently) used in a manner that facilitates a chemical reaction involving gas-liquid mass transfer to obtain solid carbon material(s). The methods described herein describe how to facilitate gas-liquid mass transfer to produce solid carbon materials in reactors that can be configured to be compatible with the methods described herein.

Without wishing to be bound by any particular theory, the processes or mechanism of gas-liquid mass transfer used herein may include three stages: (1) gas-liquid mass transfer, (2) which gives rise to chemical reactions that (3) give rise to solid carbon material( s), such as graphene-like material(s) or onion carbon (OLC). Gas-liquid mass transfer is a physical phenomenon that, under certain conditions, gives rise to chemical reactions. These reactions occur as diffusing gas molecules exchange at gas-liquid interfaces. To facilitate the production of solid carbon materials, according to embodiments herein, the gas is preferably dispersed in a liquid with small gas bubbles. Smaller bubbles create more surface area at the interface and thus give more gas-to-liquid transfer (see, for example, Sideman et al., Ind. Eng. Chem. 1966, 58, 7, 32-47). Without wishing to be bound by any particular theory, the phenomenon of "mass transfer with a chemical reaction" occurs whenever one phase contacts one or more other phases not in chemical equilibrium with them. This phenomenon is of industrial, biological and physiological importance. When creating a chemical process, it is encountered in both, separation processes and reaction creation. In some cases, a chemical reaction may be deliberately used to increase the rate of mass transfer and/or to increase the efficiency of the solvent; in other cases, a multiphase reaction system is part of a process with the express purpose of forming a product.

Without wishing to be bound by any particular theory, gas-liquid mass transfer reactors accelerate gas-to-liquid transfer by adding conditions of high pressure, heat, or extreme mixing, shear, or a combination thereof. Numerous gas-liquid mass transfer reactor technologies have been developed, some of which are trial run systems (Visscher et al., Chemical Engineering Research And Design , 2013, 91, 1923-1940), others are industrial systems such as process water treatment, liquid catalytic hydrogenation and removing CO ₂ by reacting CO ₂ gas with reactive solvents (Numerical Gas-Liquid Mass Transfer: Application In Water Treatment Process And Experimental Validation, October 1999, Conference: Second European Congress Of Chemical Engineering (Ecce2), At: Montpellier, France; Yuea et al., Chinese Academy Of Sciences, Beijing 100039, 21 December 2006 Available Online 17 January 2007, and Introduction To Modeling Of Mass Transfer Processes , PA Ramachandran, March 14, 2018).

When a gas reacts with a liquid, mass transfer occurs simultaneously with the chemical reaction. In such a situation, chemical kinetics is combined with mass movement, which means that it is no longer just a chemical reaction, but rather a complex chemical-physical process. Depending on the reactor and various operating parameters, the process tends to be diffusion rate limited or reaction rate limited. For example, the process can be thought of as first requiring the infusion of a gas into a bubble liquid that is diffusion limited, followed by a reaction at the interface of the liquid and gas bubble.

Basic chemical design theory postulates a linear relationship between the degree of agitation, shear, or mixing and the overall result ( _Ktotal ), such as in mechanically agitated reactor systems. At lower agitation rates, the process is rate-limited "diffusion", but at a certain level of agitation there is a transition zone where the result reaches a plateau and becomes rate-limited "reaction". This is illustrated in FIG. 22, for example, in the diagram K _total to rpm. stirrers from the book “Scaling Chemical Processes, Practical Guides in Chemical Engineering” by Jonathan Wostell, 2016.

It is also important to consider the degree to which the gas is soluble in the liquid. If the gas is sparingly soluble in the liquid, then the process will tend to be rate-limited by diffusion.

As will be appreciated from the foregoing and following discussions, a marked improvement in the methods and system described herein over conventional technologies for producing hard carbon materials, including but not limited to graphene and graphene-like materials, for example, is that hard carbon materials receive in the form of dispersion in situ. In other words, upon receipt and after receipt, solid carbon materials are dispersed in a liquid. In contrast, certain conventional graphene technologies, such as those using chemical vapor deposition, form graphene on or otherwise physically and/or chemically bonded to a solid substrate. According to such conventional techniques, the preparation of a graphene dispersion requires subsequently removing the graphene from said substrate and then dispersing the graphene in a liquid, thus not obtaining an in situ dispersion. Dispersions of graphene or other hard carbon materials are useful for a variety of applications including, but not limited to, lubrication. In addition, dispersions can be simpler and safer to handle than dry solid powders, even in cases where the end use requires a solid carbon material in powder form. In addition, drying or filtering the dispersion may be easier and less expensive than the chemistry required to disperse the solid powder in a solvent. Thus, the methods described herein are advantageous in that they produce in situ dispersions containing solid carbon material(s) that are produced in a single step rather than multiple steps. In an embodiment, the present invention is a dispersion containing at least one solid carbon material in a liquid, where at least one solid carbon material is produced in accordance with any of the methods described herein. Solid carbon material and liquid are described throughout the document. In some embodiments, the dispersion can be described as stable, such that particles of solid carbon material remain dispersed in the dispersion and do not precipitate or precipitate from the dispersion liquid for a specified period of time (e.g., at least 1 hour, at least 2 hours, at least 3 hours, at least 5 hours, at least 12 hours, at least 24 hours, at least 36 hours, at least 48 hours, or at least at least 1 week) at normal temperature and pressure (NTP) and under the influence of air.

Throughout the specification, hydrodynamic cavitation reactors and methods using hydrodynamic cavitation reactors are described. As is apparent from the foregoing, hydrodynamic cavitation reactors used and described herein include a subset of gas-liquid mass transfer reactors that are compatible with the methods described herein in order to prepare and functionalize solid carbon materials.

Part of a typical hydrodynamic cavitation reactor 100 used in the methods described herein is illustrated in FIG. 1. Hydrodynamic cavitation reaction 100 is a typical solid carbon material reactor, according to certain embodiments herein. The hydrodynamic cavitation reactor 100 includes a pre-cavitation chamber 102, the internal volume of which corresponds to the pre-cavitation zone 104. The pre-cavitation chamber 102 is operatively connected to the diaphragm 106. The diaphragm 106 includes an opening 110 having an opening zone 108. The diaphragm 106 is operatively connected to the cavitation chamber 112. The internal volume of the cavitation chamber 112 corresponds to the cavitation zone 114. The functional relationship between the pre-cavitation chamber 102, the diaphragm 106 and the cavitation chamber 112 allows the liquid 120, which is delivered to the pre-cavitation zone 104 from the pre-cavitation chamber 102, to flow out of the pre-cavitation zone 104 through the area of the hole 108 from the hole 110 and into the cavitation zone 114 from the cavitation chamber 112 as illustrated by the liquid flow direction arrows 122(I) and 122(II). The sudden change in pressure associated with the transition of liquid 120 from the zone of the opening 108 to the cavitation zone 114 causes the formation of cavitation bubbles 118 in the nucleation zone of the cavitation bubble 116. The cavitation zone 114, including the nucleation zone 116 of the cavitation bubble, corresponds to the "reaction zone" of the reactor. The cavitation zone 114 includes a nucleation zone 116 of the cavitation bubble. For example, cavitation bubbles are nucleated directly at the interface between opening 110 and cavitation chamber 112. Hydrodynamic cavitation reactor 100 further includes gas delivery tubes 124(I) and 124(II) to deliver gas 126 to cavitation zone 114, for example, directly to zone 116 nucleation of the cavitation bubble. Gas flow direction arrows 128(I) and 128(II) indicate the direction of gas delivery. Optionally, the reactor 100 includes one gas delivery tube or more than two gas delivery tubes. Optionally, reactor 100 includes more than one opening 110. Hydrodynamic cavitation reactors used in the methods described herein may have other configurations, including the features and configurations of hydrodynamic cavitation reactors known in the art.

Included herein is a method for producing carbon materials in situ in the cavitation cloud of a hydrodynamic cavitation reactor, without starting carbon material (eg, graphite material). This is achieved by injecting gas from the rear side (eg outlet) of the cavitation hole where cavitation bubbles form. This is essentially an additive manufacturing process where there is the formation and accumulation of new carbon material. The type, volume, size, and volume of the carbon material are collectively determined by the choice of solvents, gas, run time, gas pressure, fluid flow, and/or orifice configuration. The gas-fed reactor can also be used with graphite starting material to form additional materials or remove physical defects from existing graphene. The process can also be carried out with various gases to functionalize graphene, hexagonal boron, or other carbon-like materials. Compared to conventional processes, the methods described herein can take minutes or even seconds rather than hours, are low cost, minimally use unwanted chemicals, use less energy, and/or are highly scalable.

Hydrodynamic cavitation reactors create a cavitation cloud, which is a special environment for creating various chemical and physical reactions. Cavitation clouds occur when there is a sudden drop in pressure as a high-pressure fluid passes through a restriction such as an orifice. Cavitation clouds are composed of millions of microbubbles formed at the outlet of the hole. Cavitation bubbles go through 3 stages: 1) bubble formation, 2) very rapid bubble contraction, which creates a short-lived localized hot spot, and 3) bubble collapse, which creates an enormous amount of energy. The results of the experiment showed that when the cavitation bubbles collapse, they give internal temperatures of about 5000 K, pressures of about 14700 psi, and heating and cooling rates above 1010 K/s. These temperature and pressure changes last for less than a few nanoseconds and occur at millions of locations in the cavitation cloud (see, for example, Understanding Hydrodynamic Cavitation Report. Available from: https://www.researchgate.net/publication/314034417_Understanding_Hydrodynamic_Cavitation_Report; last accessed 28 June 2018). These intensive microreactor conditions are carried out under ambient conditions (corresponding to average bulk temperatures). In comparison, producing such a high temperature, high pressure environment in a conventional reactor can be very costly.

It has been found that when a carbon liquid, alone or in combination with a certain carbon gas, is subjected to hydrodynamic cavitation or shear, or a combination of hydrodynamic cavitation and shear, carbon materials (eg, graphene-like materials) form in situ . The method includes, inter alia , injecting the high carbon gas into the high carbon liquid extremely close to where the cavitation bubbles form, which occurs on the back side of the orifice. As used herein, the "back side" of the hole corresponds to the exit point of the hole relative to the liquid flowing through it, or, in other words, corresponds to the side of the hole that goes into the cavitation chamber or the interface between them.

It is also possible, but with much less carbon formation, to inject the gas upstream of the orifice (eg, in the pre-cavitation chamber, at/close to the interface between the orifice and the pre-cavitation chamber, and/or at the inlet of the orifice to the cavitation chamber). Without wishing to be bound by any particular theory, it is believed that the concentration of gas at the site where cavitation bubbles form maximizes the dispersion of gas in the cavitation cloud, which in turn enhances the formation of carbonaceous material.

A common method of introducing gas into a hydrodynamic cavitation reactor involves sparging or injecting gas up to the cavitation opening, which creates entrapped (absorbed or dissolved) gas. It has been found that the conventional method of introducing gas up to the orifice does not trap the adsorbed gas. Passing a liquid through an orifice actually removes gas from the liquid. This has been proven by conventional hydrodynamic cavitation reactors used for liquid degassing.

When the traditional method of bubbling acetylene into ethanol is used (i.e. before the cavitation hole), very little graphene-like material is formed. Conversely, when the gas is injected directly into the cavitation cloud behind the hole, an abundance of graphene is formed.

Moreover, since carbon materials are created in situ , it is possible to eliminate the two-stage process of creating graphene powder with subsequent redispersion of the powder in a liquid. For example, carbon plates can be formed and stored in a liquid (eg, mineral oil or propylene glycol).

A problem associated with the redispersion of graphene powder is that it is difficult to create a colloidal dispersion by conventional methods. This is because the very act of obtaining graphene powder creates a van der Waals bond between the graphene plates, which causes the graphene plates to shift. Redispersing a powder in another liquid usually requires shearing, sonication, or hydrodynamic cavitation. Even then it is difficult to obtain nano-like colloidal dispersions. In applications where graphene cannot be left in a liquid containing carbon, the graphene material can be recovered either by filtration or centrifugation.

The invention is further illustrated by the following embodiments.

(Embodiment 1) A method for producing a solid carbon material, including: delivering a liquid containing at least one liquid organic compound to a cavitation reactor; formation of cavitation bubbles in the liquid in the cavitation zone of the cavitation reactor; and delivering a gas containing at least one gaseous organic compound to the cavitation zone of the cavitation reactor; thus, obtaining a carbon material in the form of a dispersion containing a carbon material dispersed in a liquid.

(Embodiment 2) The method of Embodiment 1, wherein the cavitation reactor is a hydrodynamic cavitation reactor, a shear reactor, an ultrasonic cavitation reactor, or a multifunctional reactor.

(Embodiment 3) The method of Embodiment 2, wherein the cavitation reactor includes hydrodynamic cavitation and shear; or where the cavitation reactor includes ultrasonic cavitation and shear.

(Embodiment 4) The method of Embodiment 2, wherein the cavitation reactor includes hydrodynamic cavitation and a rotor-stator reactor; or where the cavitation reactor includes ultrasonic cavitation and a rotor-stator type reactor.

(Embodiment 5) The method of Embodiment 2, wherein the cavitation reactor includes a rotor-stator reactor, a battery shear reactor, a high speed shear reactor, a hydrodynamic cavitation reactor, a sieve reactor, a rotary packed bed reactor, a rotary disk reactor, a colliding jets, an ultrasonic gas-solid reactor, an ultrasonic reactor, an ultrasonic probe reactor, a stirred shear reactor, or a combination thereof.

(Embodiment 6) The method of any one of embodiments 1-5, wherein the gas delivery comprises gas capture, gas injection, or a combination thereof.

(Embodiment 7) The method of Embodiment 6 wherein the gas is trapped in the liquid.

(Embodiment 8) The method of Embodiment 6, wherein the gas is injected into the liquid.

(Embodiment 9) The method of Embodiment 8 wherein a gas is bubbled into a liquid.

(Embodiment 10) The method of any one of Embodiments 1 to 9, wherein the gas is delivered directly to the cavitation zone during the gas delivery step.

(Embodiment 11) The method of any one of embodiments 1 to 10, wherein the steps of cavitation bubble formation and gas delivery are performed simultaneously or nearly simultaneously.

(Embodiment 12) The method according to any one of embodiments 1 to 11, wherein during the gas delivery step, the gas is delivered directly to or within 1 mm of the cavitation bubble nucleation region, where the cavitation bubble nucleation region corresponds to the cavitation bubble nucleation in the hydrodynamic cavitation reaction during formation stage.

(Embodiment 13) The method of any one of embodiments 1 to 12, wherein the forming step includes forming a cavitation cloud containing cavitation bubbles in the cavitation zone of the reactor, where the gas is delivered directly inside or 1 mm from the cavitation cloud.

(Embodiment 14) The method according to any one of Embodiments 1 to 13, wherein the dispersion is formed in the cavitation zone of the reactor.

(Embodiment 15) The method according to any one of embodiments 1 to 14, wherein the forming step includes forming a cavitation cloud containing cavitation bubbles; where the carbon material is formed in the cavitation cloud.

(Embodiment 16) The method of any one of Embodiments 1 to 15, wherein the liquid is substantially free of carbon material during the liquid delivery step and prior to the formation of cavitation bubbles.

(Embodiment 17) The method of any one of Embodiments 1 to 16, wherein the liquid is substantially free of solid particles and is essentially no colloid, suspension, or sol during the liquid delivery step and prior to the formation of cavitation bubbles.

(Embodiment 18) The method of any one of Embodiments 1 to 17, wherein the formation of the carbon material occurs within 1 minute after the formation of cavitation bubbles in the liquid.

(Embodiment 19) The method of any one of Embodiments 1 to 18, wherein the nucleation of the carbon material occurs within 1 minute after the nucleation of the cavitation bubbles within 0.3 mm of the nucleation area of the cavitation bubbles while the gas is delivered to the cavitation zone.

(Embodiment 20) The method of any one of Embodiments 1 to 19, wherein the cavitation reactor includes a hydrodynamic cavitation reactor having a pre-cavitation zone and an orifice zone, where the orifice zone is between the pre-cavitation zone and the cavitation zone; where the hole zone includes at least one hole, such that the liquid flows from the pre-cavitation zone into the cavitation zone through at least one hole; where each of at least one hole is characterized by a hole diameter that is less than the diameter of the pre-cavitation zone.

(Embodiment 21) The method of Embodiment 20, wherein the gas is delivered directly to the cavitation end of at least one orifice or 1 mm from the end of at least one orifice; where the cavitation end of at least one hole is the end of at least one hole closest to the cavitation zone of the cavitation reactor.

(Embodiment 22) The method of any one of Embodiments 1 to 21, further comprising the step of completing delivery of gas to the cavitation zone; where the dimensional characteristic of the carbon material increases after the completion stage.

(Embodiment 23) The method of Embodiment 22, further comprising maintaining the dispersion in the cavitation zone for a time less than or equal to 60 minutes after the completion step and no gas is delivered to the cavitation zone; where the dimensional characteristic of the carbon material increases during the conservation stage.

(Embodiment 24) The method of Embodiment 23 wherein, during the step of maintaining the dispersion in the cavitation zone and after the completion step and in the absence of gas being delivered to the cavitation zone, the method further includes the step of degassing the dispersion to reduce the concentration of gas trapped therein.

(Embodiment 25) The method of any one of Embodiments 22-24, wherein the concentration of carbon material in the dispersion is substantially constant after the completion step and in the absence of gas delivery to the cavitation zone.

(Embodiment 26) The method of any one of Embodiments 1-25, further comprising recovering the solid carbon material from a dispersion in solid or powder form, wherein the recovery step comprises filtration, vacuum filtration, solvent evaporation, centrifugation, or any combination thereof.

(Embodiment 27) The method according to any one of embodiments 1-26, wherein the concentration of at least one liquid organic compound in the liquid is selected from a range of 1 wt. up to 100% wt.

(Embodiment 28) The method of Embodiment 27, wherein the concentration of solid carbon material in the dispersion is from 0.0025 wt. up to 7% wt.

(Embodiment 29) The method of any one of Embodiments 1-28, wherein at least one liquid organic compound is selected from the group consisting of a monomer, an oligomer, a prepolymer, a polymer, an organic solvent, and any combination thereof.

(Embodiment 30) The method of any one of Embodiments 1 to 29, wherein at least one liquid organic compound is selected from the group consisting of methanol, ethanol, isopropyl alcohol, methylpyrrolidone, d-cyclopentadiene, hexane, benzene, toluene, heptane, xylene, DMSO, mineral oil, machine oil, MOBILE 1™ machine oil, Syn 530 machine oil, AMSOIL™, NonSyn, QUAKER STATE™ 530 machine oil, base oil, hydrogenated castor oil, gear oil, gear oil, vegetable oil, hydrocarbon drilling fluid bases, oils with additives, oils without additives (for example, high-carbon oil), kerosene, diesel fuel, ethylene glycol, propylene glycol, diethylene glycol, triethylamine, trimethylamine, pentane, cyclopentane, cyclohexane, 1,4-dioxane, chloroform, diethyl ether, dichloromethane, tetrahydrofuran, ethyl acetate, acetone, dimethylformamide, acetonitrile, nitromethane, propylene carbonate, formic acid lots, butanol, propanol, acetic acid, octadecene, oleic acid, oleylamine, octane, diethylene glycol ether, 1,2-dichlorobenzene, methyl acetate, tetrachlorethylene, diphenylthiourea, hexafluoro-2-propanol, cinnamic acid, trimethylamine, benzenethiol, ethanethiol, ethanedithiol, 4-aminobenzenethiol, acrylic acid, carbon disulfide, 1,2-dichlorobenzene, N-methyl-2-pyrrolidone, and any combination thereof.

(Embodiment 31) The method of any one of Embodiments 1 to 30, wherein the gaseous organic compound is selected from the group consisting of methane, acetylene, ethylene, propane, 1,3-butadiene, butane, and any composition thereof.

(Embodiment 32) The method of any one of Embodiments 1 to 31, wherein the liquid has a bulk temperature of less than 400°C.

(Embodiment 33) The method of any one of Embodiments 1 to 32, wherein the gas has a bulk temperature of less than 400°C.

(Embodiment 34) The method of any one of Embodiments 1 to 33, wherein the liquid has a flow rate selected from a range of 5 L/min to 200 L/min in the cavitation zone of the cavitation reactor.

(Embodiment 35) The method of any one of Embodiments 1-34, wherein the gas is injected at a pressure characterized by a pressure selected from a range of 2 psi. up to 150 psi in the cavitation zone of the cavitation reactor.

(Embodiment 36) The method of any one of Embodiments 1-35, wherein the pressure in the cavitation zone is selected from the range of 10 psi to 10 psi. up to 5000 psi

(Embodiment 37) The method of any of Embodiments 1 to 36, wherein the cavitation reactor includes a rotor-stator, and wherein the rotor-stator operates at a rotation speed selected from a range of 200 rpm to 14,000 rpm in a cavitation zone of the cavitation reactor .

(Embodiment 38) The method of any one of Embodiments 1 to 37, wherein the residence time of the liquid in the cavitation reactor is selected from the range of 0.05 to 20 seconds.

(Embodiment 40) The method of any one of Embodiments 1-38, wherein the method is performed for a time selected from the range of 1-60 minutes.

(Embodiment 41) The method of any one of Embodiments 1-39, wherein the cavitation reactor includes an ultrasonic reactor, and wherein the ultrasonic reactor is operated at a sonication frequency of 20-300 kHz and an amplitude range of 10-100%.

(Embodiment 42) The method of any one of Embodiments 1 to 40, wherein no carbon material is produced if the method is performed without a gas delivery step under otherwise equivalent steps and conditions.

(Embodiment 43) The method of any one of Embodiments 1 to 41, wherein the dispersion or the carbon material in the dispersion has a Zeta potential greater than +40 mV or less than -160 mV.

(Embodiment 44) The method of any one of Embodiments 1 to 42, wherein the dispersion or the carbon material in the dispersion has a Zeta potential greater than +40 mV or less than -40 mV.

(Embodiment 45) The method according to any one of Embodiments 1-43, wherein the carbon concentration (atomic concentration) in the solid carbon material in the dispersion is selected from the range of 92-99 wt%.

(Embodiment 45) The method of any one of Embodiments 1-44, wherein the dispersion is a colloid, a suspension, or a combination thereof.

(Embodiment 46) The method of any one of Embodiments 1-45, wherein the carbon material comprises graphene, carbon nanotubes, carbon onions, another carbon allotrope, a composite containing graphene, or any combination thereof.

(Embodiment 47) The method of Embodiment 46, wherein the compound includes sulfur and graphene, or includes hexagonal boron nitride and graphene.

(Embodiment 48) The method of any one of Embodiments 1 to 47, wherein the carbon material comprises graphene.

(Embodiment 49) The method of Embodiment 48, wherein the carbon material is graphene.

(Embodiment 50) The method of any one of Embodiments 1 to 49, wherein the carbon material comprises a graphene polymer nanocomposite.

(Embodiment 51) The method of any one of embodiments 46-50, wherein the graphene is wrinkled graphene, crumbled graphene, holed graphene, or any combination thereof.

(Embodiment 52) The method of any one of Embodiments 1 to 51, wherein the carbon material has an oxygen content of 7 atom%. or less.

(Embodiment 53) The method of any one of Embodiments 1 to 52, further comprising using a carbon material or dispersion to reduce friction.

(Embodiment 54) The method of Embodiment 53, wherein the dispersion reduces the coefficient of friction by at least 5%.

(Embodiment 55) The method of Embodiment 53 or 54 wherein the dispersion is used to reduce friction without removing or isolating the carbon material from the dispersion.

(Embodiment 56) The method of any one of Embodiments 1 to 55, further comprising using a hard carbon material or dispersion to reinforce a battery anode and/or a battery cathode.

(Embodiment 57) The method of any one of Embodiments 1 to 56, further comprising functionalizing the carbon material to obtain a functionalized carbon material.

(Embodiment 58) The method of any one of Embodiments 1 to 57, wherein the dispersion is the first dispersion, the carbon material is the precursor material, and the cavitation reactor is the first cavitation reactor; where the method further includes: delivering the first dispersion to the second cavitation reactor; formation of cavitation bubbles in the first dispersion in the cavitation zone of the second cavitation reactor; and delivering a gas containing at least one gaseous organic compound directly to the cavitation zone of the second cavitation reactor; thereby converting the precursor material into a second carbon material, wherein the second carbon material in the form of a second dispersion comprises a second carbon material dispersed in a liquid; where the precursor material and the second carbon material are different.

(Embodiment 59) The method of Embodiment 58, wherein the first hydrodynamic cavitation reactor and the second hydrodynamic cavitation reactor are the same.

(Embodiment 60) A method for functionalizing a material dispersed in a liquid, wherein the material is dispersed in a liquid being a first dispersion, wherein the method includes the steps of: delivering the first dispersion to a cavitation reactor; where the liquid contains at least one liquid organic compound; formation of cavitation bubbles in the liquid in the cavitation zone of the cavitation reactor; and delivering a gas containing at least one gaseous organic compound directly to the cavitation zone of the cavitation reactor; thus functionalizing the material to form a second dispersion, wherein the second dispersion contains the functionalized material dispersed in a liquid.

(Embodiment 61) The method of Embodiment 60, wherein the functionalization of the material includes chemical, physical, or both chemical and physical functionalization of the material.

(Embodiment 62), The method of Embodiment 60 or Embodiment 61, wherein the material comprises graphite, expanded graphite, graphite-like material, graphene, graphene-like material, carbon nanotubes, carbon onions, another carbon allotrope, graphene-containing composite, cationic graphene, or any combination of them.

(Embodiment 63) The method of any one of Embodiments 60-62, wherein the functionalized material comprises graphene oxide.

(Embodiment 64) The method of any one of embodiments 60-63, wherein the functionalization comprises adding oxygen atoms to the material, removing oxygen atoms from the material, adding nitrogen atoms to the material, adding sulfur atoms to the material, or a combination thereof.

(Embodiment 65) The method of any of embodiments 60-64, wherein the gas comprises oxygen, steam, hydrogen, nitrogen, sulfur dioxide, CO ₂ , or any combination thereof.

(Embodiment 66) A functionalized material obtained by the method of any one of Embodiments 60-65.

The invention is further illustrated by the following additional embodiments:

(Embodiment 101) A method for producing a solid carbon material, including: delivering a liquid containing at least one liquid organic compound to a reaction zone of a reactor; delivering a gas containing at least one gaseous organic compound to the reaction zone of the reactor; and inducing a chemical reaction between at least one liquid organic compound and at least one gaseous organic compound, where: the chemical reaction occurs in the reaction zone of the reactor; solid carbon material obtained through a reaction; the solid carbon material is obtained during the reaction in the form of a dispersion comprising the solid carbon material dispersed in a liquid; and the chemical reaction is a homogeneous reaction involving homogeneous nucleation of solid carbon material in the reaction zone of the reactor.

(Embodiment 102) The method of Embodiment 101, wherein the chemical reaction comprises gas-liquid mass transfer.

(Embodiment 103) The method of any one of embodiments 101-102, wherein the gas composition is different from the liquid composition.

(Embodiment 104) The method of any one of embodiments 101-103, wherein the composition of at least one gaseous complex is different from that of at least one liquid organic compound.

(Embodiment 105) The method of any one of embodiments 101-104, wherein the chemical reaction does not occur on or in the catalyst.

(Embodiment 106) The method of any one of embodiments 101-105, wherein the method does not include heterogeneous nucleation of a solid carbon material crystal on a solid support.

(Embodiment 107) The method of any one of embodiments 101-106, wherein the step of delivering liquid is performed via the first inlet to the reaction zone, and the step of delivering gas is performed via the second inlet to the reaction zone; where the paths of the first stream and the second input stream are different and are physically separate.

(Embodiment 108) The method of any one of embodiments 101-107, wherein the liquid delivery step and the gas delivery step are performed simultaneously.

(Embodiment 109) The method of any one of embodiments 101-107, wherein the gas delivery step is performed after the liquid is delivered to the reaction zone.

(Embodiment 110) The method of any one of embodiments 101-109 wherein the solid carbon material remains dispersed in the liquid while in the reaction zone.

(Embodiment 111) The method of any one of embodiments 101-110, wherein the liquid is substantially free of solid carbon material during the liquid delivery step and up to the gas delivery and chemical reaction induction steps.

(Embodiment 112) The method of any one of embodiments 101-111, wherein the liquid is substantially free of solid particles and substantially free of colloid, suspension, or sol during the liquid delivery step and up to the gas delivery and chemical reaction induction steps.

(Embodiment 113) The method of any one of embodiments 101-112, wherein the solid carbon material is only formed in the reaction zone of the reactor.

(Embodiment 114) The method of any one of embodiments 101-113, wherein no solid carbon material is produced when the method is performed without the step of performing gas delivery under other equivalent steps and conditions.

(Embodiment 115) The method of any one of embodiments 101-114, wherein the gas delivery comprises gas capture, gas injection, or a combination thereof.

(Embodiment 116) The method of Embodiment 115 wherein the gas is entrained in a liquid under pressure.

(Embodiment 117) The method of Embodiment 115, wherein the gas is injected into the liquid.

(Embodiment 118) The method of Embodiment 115 wherein the gas is bubbled into the liquid.

(Embodiment 119) The method of any one of Embodiments 101-18, wherein the gas is delivered directly to the reaction zone during the gas delivery step.

(Embodiment 120) The method of any one of embodiments 101-119, wherein the steps of delivering the gas and inducing a chemical reaction are performed simultaneously or nearly simultaneously.

(Embodiment 121) The method of any one of embodiments 101-120, wherein at least one liquid organic compound and at least one gaseous organic compound are simultaneously present in the reaction zone.

(Embodiment 122) The method of any one of embodiments 101-121, wherein the reactor includes a mechanically stirred reactor, a turbine reactor, a monolithic reactor, a foam reactor, a rotor-stator reactor, a shear stack reactor, a high-speed shear reactor (e.g., Charles Ross HSM-700), Hydrodynamic Cavitation Reactor, Sieve Reactor, Tubular Rotary Reactor, Packed Bed Rotary Reactor, Accordion Type Rotary Reactor, Fluidized Bed Reactor, Taylor-Couette Reactor, Double Tube Reactor, Rotary Disk Reactor, Colliding Jet Reactor , ultrasonic gas-solid reactor, ultrasonic reactor, ultrasonic probe reactor, microwave reactor, shock wave reactor (e.g. SHOCKWAVE POWER™ Reactor (SPR)), continuous flow reactor (e.g. RAPTOR™ reactor), stirred reactor , providing a shift or a combination of them.

(Embodiment 123) The method of any one of embodiments 101-122, wherein the step of inducing a chemical reaction comprises inducing a shear force in the fluid.

(Embodiment 124) The method of Embodiment 123, wherein the reactor is a mechanically stirred reactor including a stirrer; and where the agitator induces a shear force in the fluid.

(Embodiment 125) The method of Embodiment 124, wherein the agitator is selected from the group consisting of a gas-inducing agitator, a Rushton agitator/turbine, a monolithic agitator, a helical agitator, a plate or radial flat impeller, an axial propeller, an angled blade, a turbine vortex mixer, several mixers on one rod and any combination thereof.

(Embodiment 126) The method of Embodiment 125, wherein the agitator is a gas-inducing agitator.

(Embodiment 127) The method of any one of embodiments 124-126, wherein the agitator has a rotation speed selected from the range of 200-14000 rpm.

(Embodiment 128) The method of any one of embodiments 124-127, wherein the step of inducing a chemical reaction comprises stirring or mixing a liquid and a gas in the reaction zone.

(Embodiment 129) The method of any one of Embodiments 123-128, wherein the pressure in the reactor zone is selected from the range of 6 bar (about 87 psi) to 150 bar (about 2175 psi). ).

(Embodiment 130) The method of any one of Embodiments 123-129, wherein the temperature in the reaction zone is selected from the range of 20°C to 250°C.

(Embodiment 131) The method of any one of embodiments 101-122, wherein: the reactor is a cavitation reactor; the reaction zone is the cavitation zone of the cavitation reactor; and the method includes forming cavitation bubbles in the liquid in the cavitation zone of the cavitation reactor.

(Embodiment 132) The method of Embodiment 131, wherein the cavitation reactor is a hydrodynamic cavitation reactor, a shear reactor, an ultrasonic cavitation reactor, or a multifunctional reactor.

(Embodiment 133) The method of Embodiment 132, wherein the cavitation reactor includes hydrodynamic cavitation and shear; or where the cavitation reactor includes ultrasonic cavitation and shear.

(Embodiment 134) The method of Embodiment 132, wherein the cavitation reactor includes hydrodynamic cavitation and a rotor-stator reactor; or where the cavitation reactor includes ultrasonic cavitation and a rotor-stator type reactor.

(Embodiment 135) The method of Embodiment 132, wherein the cavitation reactor includes a rotor-stator reactor, a shear stack reactor, a high speed shear reactor, a hydrodynamic cavitation reactor, a sieve reactor, a rotary packed bed reactor, a rotary disk reactor, a colliding jets, an ultrasonic gas-solid reactor, an ultrasonic reactor, an ultrasonic probe reactor, a microwave reactor, a shock wave reactor, a stirred shear reactor, or a combination thereof.

(Embodiment 136) The method of any one of embodiments 131-135, wherein the gas is delivered directly to the cavitation zone during the gas delivery step.

(Embodiment 137) The method of any one of embodiments 131-136, wherein the steps of cavitation bubble formation and gas delivery are performed simultaneously or nearly simultaneously.

(Embodiment 138) The method of any one of embodiments 131-137, wherein during the gas delivery step, the gas is delivered directly to or within 1 mm of the cavitation bubble nucleation region, where the cavitation bubble nucleation region corresponds to the cavitation bubble nucleation in the hydrodynamic cavitation reaction during formation stage.

(Embodiment 139) The method of any one of embodiments 131-138, wherein the forming step includes forming a cavitation cloud including cavitation bubbles in the cavitation zone of the reactor, where the gas is delivered directly inside or 1 mm from the cavitation cloud.

(Embodiment 140) The method of any one of embodiments 131-139, wherein the forming step includes forming a cavitation cloud including cavitation bubbles; where the carbon material is formed in the cavitation cloud.

(Embodiment 141) The method of any one of embodiments 131-140, wherein the liquid is substantially free of carbon material during the liquid delivery step and prior to the formation of cavitation bubbles.

(Embodiment 142) The method of any one of embodiments 131-141, wherein the liquid is substantially free of solid particles and is substantially free of colloid, suspension, or sol during the liquid delivery step and prior to the formation of cavitation bubbles.

(Embodiment 143) The method of any one of embodiments 131-142, wherein the formation of the carbon material occurs within 1 minute after the formation of cavitation bubbles in the liquid.

(Embodiment 145) The method of any one of embodiments 131-143, wherein the nucleation of the carbon material occurs within 1 minute after the nucleation of the cavitation bubble crystal within 0.3 mm of the cavitation bubble nucleation area while the gas is delivered to the cavitation zone.

(Embodiment 146) The method of any one of embodiments 131-144, wherein the cavitation reactor includes a hydrodynamic cavitation reactor having a pre-cavitation zone and an orifice zone, where the orifice zone is between the pre-cavitation zone and the cavitation zone; the hole zone includes at least one hole, such that liquid flows from the pre-cavitation zone into the cavitation zone through at least one hole; where each of at least one hole is characterized by a hole diameter that is less than the diameter of the pre-cavitation zone.

(Embodiment 146) The method of Embodiment 145, wherein the gas is delivered directly to the cavitation end of at least one orifice or 1 mm from the end of at least one orifice; where the cavitation end of at least one hole is the end of at least one hole closest to the cavitation zone of the cavitation reactor.

(Embodiment 147) The method of any one of embodiments 131-146, further comprising the step of completing delivery of gas to the cavitation zone; where the dimensional characteristic of the carbon material increases after the completion stage.

(Embodiment 148) The method of Embodiment 147, further comprising maintaining the dispersion in the cavitation zone for a time less than or equal to 60 minutes after the completion step and no gas being delivered to the cavitation zone; where the dimensional characteristic of the carbon material increases during the conservation stage.

(Embodiment 149) The method of Embodiment 148, wherein, during the step of maintaining the dispersion in the cavitation zone and after the completion step and in the absence of gas delivery to the cavitation zone, the method further includes the step of degassing the dispersion to reduce the concentration of gas trapped therein.

(Embodiment 150) The method of any one of embodiments 147-149, wherein the concentration of carbon material in the dispersion is substantially constant after the completion step and in the absence of gas delivery to the cavitation zone.

(Embodiment 151) The method of any one of embodiments 101-50, further comprising recovering the solid carbon material from a dispersion in solid or powder form, wherein the recovery step includes filtration, vacuum filtration, solvent evaporation, centrifugation, or any combination thereof.

(Embodiment 152) The method of any one of embodiments 101-121, wherein the concentration of at least one liquid organic compound in the liquid is selected from a range of 0.01 wt. up to 100% wt.

(Embodiment 153) The method of any one of embodiments 101-152, wherein at least one liquid organic compound is selected from the group consisting of a monomer, an oligomer, a prepolymer, a polymer, an organic solvent, and any combination thereof.

(Embodiment 154) The method according to any one of embodiments 101-153, at least one liquid organic compound is selected from the group consisting of methanol, ethanol, isopropyl alcohol, methylpyrrolidone, d-cyclopentadiene, hexane, benzene, toluene, heptane, xylene, DMSO, mineral oil, machine oil, MOBILE 1™ machine oil, Syn 530 machine oil, AMSOIL™, NonSyn, QUAKER STATE™ 530, base oil, hydrogenated castor oil, gear oil, gear oil, vegetable oil, drilling oil solution, oils with additives, oils without additives (for example, high-carbon oil), kerosene, diesel fuel, ethylene glycol, propylene glycol, diethylene glycol, triethylamine, trimethylamine, pentane, cyclopentane, cyclohexane, 1,4-dioxane, chloroform, diethyl ether, dichloromethane, tetrahydrofuran, ethyl acetate, acetone, dimethylformamide, acetonitrile, nitromethane, propylene carbonate, formic acid ota, butanol, propanol, acetic acid, octadecene, oleic acid, oleylamine, octane, diethylene glycol ether, 1,2-dichlorobenzene, methyl acetate, tetrachlorethylene, diphenylthiourea, hexafluoro-2-propanol, cinnamic acid, trimethylamine, benzenethiol, ethanethiol, ethanedithiol, 4-aminobenzenethiol, acrylic acid, carbon disulfide, 1,2-dichlorobenzene, N-methyl-2-pyrrolidone, and any combination thereof.

(Embodiment 155) The method of any one of Embodiments 101-154, wherein the liquid comprises water.

(Embodiment 156) The method of any one of embodiments 101-155, wherein the gaseous organic compound is selected from the group consisting of methane, acetylene, ethylene, propane, 1,3-butadiene, butane, and any combination thereof.

(Embodiment 157) The method of any one of Embodiments 101-156, wherein the liquid has a bulk temperature of less than 400°C.

(Embodiment 158) The method of any one of Embodiments 101-157, wherein the liquid has a bulk temperature of 20°C or more.

(Embodiment 159) The method of any one of Embodiments 101-158, wherein the gas has a bulk temperature of less than 400°C.

(Embodiment 160) The method of any one of Embodiments 101-159, wherein the gas has a bulk temperature of 20°C or more.

(Embodiment 161) The method of any one of embodiments 101-160, wherein the liquid has a flow rate selected from the range of 5 L/min to 200 L/min in the cavitation zone of the cavitation reactor.

(Embodiment 162) The method of any one of embodiments 101-161, wherein the gas is injected at a pressure characterized by a pressure selected from a range of 2 psi. up to 150 psi in the reaction zone of the reactor.

(Embodiment 163) The method of any one of Embodiments 101-162, wherein the pressure in the reaction zone is selected from the range of 10 psi. up to 5000 psi

(Embodiment 164) The method of any one of embodiments 101-163, wherein the reactor includes a rotor-stator, and wherein the rotor-stator operates at a rotation speed selected from a range of 200 rpm to 14,000 rpm in the reaction zone of the reactor.

(Embodiment 165) The method of any one of embodiments 101-064, wherein the residence time of the liquid in the reaction zone is selected from the range of 1-60 minutes.

(Embodiment 166) The method of any one of embodiments 101-165, wherein the method is performed for a time selected from the range of 1-60 minutes.

(Embodiment 167) The method of any one of embodiments 101-166, wherein the reactor includes an ultrasonic reactor, and wherein the ultrasonic reactor is operated at a sonication frequency of 20-300 kHz and an amplitude range of 10-100%.

(Embodiment 168) The method of any one of Embodiments 101-167, wherein the dispersion or carbon material in the dispersion has a Zeta potential greater than +40 mV or less than -160 mV.

(Embodiment 169) The method of any one of Embodiments 101-168, wherein the dispersion or the carbon material in the dispersion has a Zeta potential greater than +40 mV or less than -40 mV.

(Embodiment 170) The method according to any one of embodiments 101-169, wherein the concentration of solid carbon material in the dispersion is from 0.0025 wt. up to 7% wt.

(Embodiment 171) The method of any one of Embodiments 101-170, wherein the dispersion is a colloid, a suspension, a sol, or a combination thereof.

(Embodiment 172) The method of any one of embodiments 101-171, wherein the solid carbon material comprises graphite , expanded graphite, graphite-like material, graphene, graphene-like material, carbon flakes, carbon nanotubes, carbon onions, other carbon allotrope, graphene-containing composite , cationic graphene, or any combination thereof.

(Embodiment 173) The method of Embodiment 172, wherein the compound includes sulfur and graphene, or includes hexagonal boron nitride and graphene.

(Embodiment 174) The method of any one of Embodiments 101-172, wherein the carbon material comprises graphene or a graphene-like material.

(Embodiment 175) The method of Embodiment 172, wherein the carbon material is graphene or a graphene-like material.

(Embodiment 176) The method of any one of Embodiments 101-172, a carbon material comprising a graphene polymer nanocomposite.

(Embodiment 177) The method of any one of embodiments 172-176, wherein the graphene is wrinkled graphene, crumbled graphene, holed graphene, or any combination thereof.

(Embodiment 178) The method of any one of Embodiments 101-177, wherein the carbon material has an oxygen content of less than 7 atom%.

(Embodiment 179) The method of any one of embodiments 101-178, wherein the dispersion has a coefficient of friction that is reduced by at least 5% relative to the same fluid without solid carbon material.

(Embodiment 180) The method of any one of Embodiments 101-179, wherein the dispersion has a wear track reduced by at least 3% relative to the same fluid without solid carbon material.

(Embodiment 181) The method of any one of Embodiments 101-180, further comprising using a hard carbon material or dispersion to reduce friction.

(Embodiment 182) The method of any one of Embodiments 101-181, comprising reducing friction in situ.

(Embodiment 183) The method of Embodiment 181 or 182 wherein the dispersion is used to reduce friction without removing or isolating the hard carbon material from the dispersion.

(Embodiment 184) The method of any one of embodiments 101-180, further comprising using a hard carbon material or dispersion to reinforce a battery anode and/or a battery cathode.

(Embodiment 185) The method of any one of Embodiments 101-184, further comprising functionalizing the hard carbon material to obtain a functionalized hard carbon material.

(Embodiment 186) The method of any one of embodiments 101-185, wherein the dispersion is the first dispersion, the chemical reaction is the first chemical reaction, the solid carbon material is the precursor material, the gas is the first gas, and the reactor is the first reactor; where the method further includes: delivering the first dispersion to the second reactor; delivering a second gas containing at least one gaseous organic compound directly to the reaction zone of the second reactor; and inducing a second chemical reaction in the reaction zone of the second reactor; where: the second chemical reaction converts the precursor material into a second solid carbon material; the second carbon material is dispersed in the liquid; and the precursor material and the second carbon material are different.

(Embodiment 187) The method of Embodiment 186, wherein the second reactor is a cavitation reactor and the induction step includes forming cavitation bubbles in the first dispersion in the reaction zone of the second reactor.

(Embodiment 188) The method of any one of Embodiments 186-187, wherein the first reactor and the second reactor are the same.

(Embodiment 189) A method for functionalizing a first solid carbon material dispersed in a liquid, wherein the first solid carbon precursor material is dispersed in a liquid being the first dispersion, wherein the method includes the steps of: delivering the first dispersion to a reaction zone of the reactor; where the liquid contains at least one liquid organic compound; delivery of gas to the reaction zone of the reactor; and inducing a functionalization chemical reaction, wherein: the functionalization chemical reaction forms a second carbon material from the first carbon material; the functionalization chemical reaction takes place in the reaction zone of the reactor; and the second solid carbon material is obtained during the reaction in the form of a second dispersion, where the second dispersion includes a second solid carbon material dispersed in a liquid.

(Embodiment 190) The method of Embodiment 189, wherein the functionalization chemical reaction comprises chemical, physical, or both chemical and physical functionalization of the first solid carbon material.

(Embodiment 191) The method of Embodiment 189 or Embodiment 190, wherein the first solid carbon material comprises graphene oxide, graphite , expanded graphite, graphite-like material, graphene, graphene-like material, carbon slabs, carbon nanotubes, carbon onions, another carbon allotrope, a composite containing graphene, cationic graphene, or any combination thereof.

(Embodiment 192) The method of any one of embodiments 189-191, wherein the second solid carbon material comprises, reduced graphene oxide, graphene oxide, edge-oxidized graphene, graphite , expanded graphite, graphite-like material, graphene, graphene-like material, carbon flakes, carbon nanotubes, carbon onions, other carbon allotrope, composite containing graphene, cationic graphene, or any combination thereof.

(Embodiment 193) The method of any one of embodiments 189-192, wherein the first carbon solid material comprises graphene oxide and the second carbon solid material comprises reduced graphene oxide.

(Embodiment 194) The method of Embodiment 193, wherein the atomic fraction of oxygen in the second carbon material is at least 50% less than the atomic fraction of oxygen in the first carbon material.

(Embodiment 195) The method of any one of embodiments 189-192, wherein the functionalization chemical reaction comprises oxidizing the first solid carbon material such that the second solid carbon material is soluble in water.

(Embodiment 196) The method of embodiments 195, wherein the liquid comprises water and the second dispersion is an aqueous dispersion of the second carbon material in water.

(Embodiment 197) The method of any one of embodiments 189-196, wherein the functionalization chemical reaction comprises adding oxygen atoms to the first solid carbon material, removing oxygen atoms from the first solid carbon material, adding carbon atoms to the first solid carbon material, adding nitrogen atoms to the first solid carbon material, adding sulfur atoms to the first solid carbon material, or a combination thereof.

(Embodiment 198) The method of any one of embodiments 189-197, wherein the gas comprises oxygen, steam, hydrogen, nitrogen, sulfur dioxide, CO ₂ , ozone, or any combination thereof.

(Embodiment 199) The method of any one of embodiments 189-198, wherein: the reactor is a cavitation reactor and the reaction zone is a cavitation zone; the method includes the formation of cavitation bubbles in the liquid in the cavitation zone of the cavitation reactor; and the gas is injected directly into the cavitation zone.

(Embodiment 200) The method of any one of embodiments 189-199, wherein the first solid carbon material is not chemically bonded to the solid support during the functionalization chemical reaction.

(Embodiment 201) The method of any one of Embodiments 1-200, wherein the gas contains at least one gaseous organic compound.

(Embodiment 202) The method of any one of embodiments 189-200, wherein the gaseous organic compound is selected from the group consisting of alkane, alkene, alkyne, cycloalkane, heterocycloalkane, arene, heteroarene, and combinations thereof, wherein alkane, alkene, alkyne, cycloalkane , heterocycloalkane, arene or heteroarene is optionally substituted with one or more substituents.

(Embodiment 203) The method of any one of embodiments 189-202, wherein at least one gaseous organic compound is selected from the group consisting of methane, acetylene, ethylene, propane, 1,3-butadiene, butane, and any combination thereof.

(Embodiment 204) A functionalized material obtained by the method of any one of Embodiments 189-203.

The following examples further illustrate the invention, but are of course not to be construed as limiting its scope in any way.

EXAMPLE 1

This example demonstrates methods for producing one or more carbonaceous materials in a liquid using a hydrodynamic cavitation reactor. In more detail, this example represents a method for synthesizing carbon material in the cavitation cloud of a hydrodynamic cavitation reactor. a typical embodiment of the method includes: (a) flowing a high carbon liquid (a liquid including an organic compound) through a hydrodynamic cavitation reactor and then (b) introducing a high carbon gas (a gas including an organic compound) at the back of the cavitation hole at the start of nucleation of the cavitation bubbles. Within seconds, graphene-like materials begin to form in the cavitation cloud. (c) After a predetermined time, the gas flow is stopped, which inhibits the continued formation of the synthesized gaseous material. The gas pressure and flow time determine the thickness and size of the initial graphene plates. (d) Optionally, the liquid containing the graphene-like material can be left to circulate for an additional time (eg, 15 minutes). During this additional circulation time, as a result of gas entrainment, carbon material continues to form. It has been found that entrapped gas injected at the rear side (eg outlet) of a diaphragm behaves differently than entrapped gas introduced in front of the orifice; namely, the gas after the hole is not degassed as easily as the gas injected before the hole. This is confirmed by the fact that when the gas is sparged or directly injected in front of the orifice, a minimum amount of carbonaceous material is formed. However, if the liquid containing the gas induced after the orifice is left to circulate (in the absence of gas injection), additional formation of carbon material occurs.

After gas delivery is complete and the dispersion continues to circulate in the cavitation zone, the liquid may optionally be degassed. Upon degassing, the shear forces experienced by the particles of carbon material in the dispersion may result in a decrease in one or more of the dimensional characteristics of the particles. Without outgassing, the shear forces experienced by the particles of carbon material in the dispersion can lead to an increase in one or more dimensional characteristics of the carbon material in the dispersion (eg, larger and/or thicker graphene slabs). For example, increased shear forces can shrink graphene lamellae. Gas trapped in the liquid while the dispersion is subjected to shear forces or increased shear forces can make smaller lamellae thinner. A reduced concentration of entrained gas (eg, through degassing) can prevent thickening of the plates in this mode (ie, keeping the dispersion in the cavitation zone without gas delivery).

EXAMPLE 2

This example demonstrates methods for functionalizing one or more materials, such as carbon materials, using a hydrodynamic cavitation reactor. For example, the methods of this example can be used to functionalize graphene. It is possible to functionalize carbon materials obtained by the process described herein, or carbon materials obtained by other methods. Examples of such functionalization include: 1) correction of physical defects, 2) chemical functionalization with different gases, and 3) physical functionalization (eg, changing the morphology of graphene).

Correcting Defects: Correcting physical defects in graphene wafers is one of the biggest challenges in the production of pure graphene. A common approach to "correcting" graphene defects is to use CVD (chemical vapor deposition) to fill graphene wafers with a carbon-rich gas such as ethylene. The carbon in the gas effectively fills the defects. The CVD method, however, is not easily scalable.

The processes described herein can be used to add carbon to graphene to correct, or repair, defects in graphene. This has been demonstrated by forming graphene with a large number of defects and then functionalizing it to fix/fix/fill the defects with high carbon gas. For example, defective graphene is obtained by starting with graphene oxide and then reducing oxygen on the graphene by treating the graphene oxide with harsh chemicals (eg, sodium borohydride, sulfuric acid) at extremely high temperatures (eg, 1100°C). This creates a highly defective, highly reduced graphene oxide (rGO), which is then dispersed in ethanol. The dispersion is then circulated through a hydrodynamic cavitation reactor, while acetylene is injected into the cavitation cloud at the back of the orifice. Acetylene gas "fills" voids in defective graphene, which is confirmed by a noticeable increase in the conductivity of "filled" graphene on the filter washer. See FIG. 2. By comparison, filter washers of similar weight are produced with untreated high oxygen GO and deoxidized, highly reduced GO with defects. As seen from FIG. 2, there is a noticeable difference in conductivity between the three filter beads: 1) untreated graphene with low oxygen content, 2) the same graphene after deoxidation (i.e. with defects), and 3) deoxidized graphene treated with acetylene, i.e. "embedded" in an embodiment of the method of the invention.

Chemical Functionalization: The methods described herein can also be applied to the chemical functionalization of graphene and other carbon materials through the introduction of various gases into the cavitation cloud. For example, oxygen can be added to a graphene dispersion to produce graphene oxide, argon and/or hydrogen can be added to reduce oxygen on graphene wafers, nitrogen can increase the lubricity of graphene, and sulfur dioxide can add sulfur to graphene and other carbon materials.

Physical functionalization: Various combinations of gas pressure and back pressure can be used to create, for example: wrinkled graphene, crushed graphene, or graphene with holes. In addition, different combinations of gas and solvent at different pressures and with different orifices can be used to create carbon nanotubes, carbon onions, or other carbon allotropes.

EXAMPLE 3

In this example, graphene plates are formed according to certain methods described in this document. FIG. 3 shows a scanning electron microscopy (SEM) image of some graphene-like plates. FIG. 4 shows dispersive X-ray spectroscopy (EDS) energy data measured from the two portions of the plates shown in FIG. 3. Top white square and bottom white square in the SEM image of FIG. 3 correspond to "Spectrum 5" and "Spectrum 6" of the EDS plot data in FIG. 4. The atomic compositions derived from the EDS data corresponding to these graphene sheets are summarized in Table 1. In Table 1, "C/O" corresponds to the ratio of atomic concentrations of carbon to oxygen.

Table 1

Spectrum label Concentration
C (% atom) Concentration
O (% atom) Total
Concentration (% atom) C/O Ratio Spectrum 5 99.43 0.57 100.00 ~175:1 Spectrum 6 99.60 0.40 100.00 ~249:1

FIG. 5A and 5B show additional images of exemplary graphene-like wafers produced according to embodiments of the methods described herein.

EXAMPLE 4A

In this example, a carbon material containing a graphene-like material is produced using hydrodynamic cavitation according to embodiments of the methods described herein.

FIG. 6A-7B, the carbon material is produced using propane as the delivered gaseous organic compound and toluene as the liquid organic compound. FIG. 6A shows an SEM image of micron graphene wafers with squares (labeled "1" and "2") identifying regions corresponding to the EDS spectra shown in FIG. 6B (square 1 corresponds to "Spectrum 1" and square 2 corresponds to "Spectrum 2"). FIG. 6B shows the EDS spectra and Table 2 summarizes the atomic concentrations of the elements calculated from the EDS spectra in the carbon material in the regions identified in FIG. 6A.

table 2

Spectrum Label Concentration
C (% atom) O concentration
(% atom) Total
Concentration (% atom) Spectrum 1 99.19 0.81 100.00 Spectrum 2 98.23 1.77 100.00

FIG. 7A shows an SEM image of micron graphene wafers with regions (labeled "5" and "6") identifying regions corresponding to the EDS spectra shown in FIG. 7B (square 5 corresponds to "Spectrum 5" and square 6 corresponds to "Spectrum 6"). FIG. 7B shows the EDS spectra and a table summarizing the atomic concentrations of elements calculated from the EDS spectra in the carbon material in the regions defined in FIG. 7A. The carbon material formed in this example corresponding to FIG. 6A-7B has an oxygen concentration of less than 1.77 atom%. or not less than 0.40%.

In this example, a 5 mm orifice with an injection gas pressure of 3000 psi is used and the process is carried out for 1 minute.

EXAMPLE 4B

In this example, a carbon material including graphene is produced using hydrodynamic cavitation, according to embodiments of the methods described herein.

FIG. 8A-8B, the carbon material is produced using acetylene as the delivered gaseous organic compound and liquid ethanol as the liquid organic compound. In this example, the liquid is wholly or essentially an organic compound (ethanol). FIG. 8A-8B show SEM images of carbon material. In this example, a 0.5 mm orifice and an injection gas pressure of 3000 psi are used and the process is performed for 5 minutes.

Other examples of hydrodynamic reactors may be: 1) a shock wave reactor such as the SHOCKWAVE POWER™ Reactor (SPR) (Hydro Dynamics, Inc., Rome, GA). As the liquid passes through the shock wave reactor, it undergoes "controlled cavitation". The heart of the device is a specially designed rotor that rotates. Rotation creates hydrodynamic cavitation in rotor cavities away from metal surfaces. Cavitation is controlled and therefore there is no damage. When microscopic cavitation bubbles form and collapse, shock waves are emitted into the liquid, which can heat and/or mix. 2) Another hydrodynamic reactor is the rotating disk reactor. A shock wave reactor is a device that uses a rotating disk, usually close to a stationary surface, to accelerate the flow in a centrifugal manner. The components of which activate the flow (which is usually a liquid) to mix, mix, shear, create cavitation (vacuum) and produce a change in temperature, influenced by the rotation of the boundary layer. One of the main mechanisms is ultrasonic chemistry (producing ultrasound through the formation of acoustic cavitation in liquids - which leads to chemical activity). For example, when water is cavitated, there is an energy blast involving ultraviolet light, heat, and sound known as a shock wave.

EXAMPLE 5A

In this example, carbon material, including graphene, is produced using shear, according to embodiments of the methods described herein. In this example, a battery shear mixer, specifically a Fuko FM300 high shear battery system, is used as the cavitation reactor, propane is used as the delivered gaseous organic compound, MOBILE 1™ engine oil is used as the liquid organic compound. In this example, the liquid is wholly or essentially an organic compound (MOBILE 1™). The synthesis process is carried out for 2 minutes at a gas entrainment pressure of 30 psi. The gas is entrained in liquid in a separate pressure tank where the gas is injected at 30 psi. This keeps the gas in the liquid. Under atmospheric pressure, the gas is not trapped in the lubricating oil. The gas injection flow rate is 11 ml/min and a 12000 rpm shear mixer is used.

FIG. 9A shows light scattering intensity versus particle diameter, and FIG. 9B shows a corresponding table summarizing the data in FIG. 9A. The data correspond to particles of carbon material in dispersion, formed according to this example. The particle size ranges from approximately 4.4 nm to 184 nm (hydrodynamic diameter) according to dynamic light scattering. FIG. 10A shows the quantitative particle size distribution, and FIG. 10B shows a table summarizing the distribution corresponding to the carbon material particles obtained according to this example. The particles were predominantly crystalline and range in size from 1.5 to 10.8 nm.

The following description of the characterization procedures applies to Examples 5A and 5B:

.Particles suspended in liquids are in Brownian motion due to random collisions with solvent molecules. This movement causes the particles to diffuse through the medium. The diffusion coefficient, D, is inversely proportional to particle size according to the Stokes-Einstein equation:

.

Where D is the diffusion constant, kB is the Boltzmann constant, T is the absolute temperature, ƞ ₀ is the viscosity, and d is the diameter of the spherical particle.

Photon correlation spectroscopy, sometimes also called dynamic light scattering, is a technique used to determine the diffusion coefficient of small particles in a liquid. The coefficient is determined by accurately measuring the light scattering intensity of the particles as a function of time. As the particles of interest diffuse through the sample cell due to Brownian motion, the incident laser light beam irradiates the particles. Particles scatter light, producing fluctuations in scattering intensity as a function of time. Scattered light is collected at a selected angle and measured with a highly sensitive sensor. Since the rate of diffusion of particles is determined by their size, information about their size is contained in the rate of oscillation of light scattering. The intensity fluctuations are collected as photon pulses and correlated to create an autocorrelation function (ACF). The diffusion coefficient is determined by fitting the ACF using the Cumulants method, from which the average size is obtained using the Stokes-Einstein equation.

Zeta Potential: The process described herein produces crystalline particles with a very high Zeta potential. Thus, particles of carbon material, such as graphene particles, in the form of a lubricant, form a very stable dispersion, for example, having a Zeta potential of -63 mV. It is recognized in the art that a colloidal distribution having a Zeta potential greater than +40 mV or less than -40 mV is very stable.

The zeta potential is a measure of the electric potential in the glide plane in the double layer surrounding a particle suspended in solution. The double layer consists of a Stern layer and a diffuse layer. In the Stern layer, ions with the opposite charge of surface particles are attracted to the particle. As the distance from the particle surface increases, oppositely charged ions become more diffuse. The point where the ions begin to diffuse into the environment is called the slip plane, since the strongly attracted ions will move with the particle in Brownian motion. The zeta potential is measured on the glide plane. The zeta potential can be used as a measure of the stability of a particle in solution. Particles with a Zeta potential greater than +40 mV or less than -40 mV are considered stable because the charge prevents the particles from agglomerating. Conversely, particles with a Zeta potential closer to 0 mV, the isoelectric point, tend to collide and form large agglomerates.

.Electrophoretic light scattering is a technique used to determine the Zeta potential of charged particles in solution. Slip plane charge cannot be measured directly on the DELSA™ Nano C particle analyzer (Beckman Coulter, Brea, CA). Instead, the Zeta potential is determined through theoretical models and electrophoretic mobility. An electric field is applied to particles in solution. The particles will move towards the oppositely charged electrode. The particles are irradiated with laser light and scattered due to particle motion. The detected scattered light creates a frequency shift from the incident laser beam. The frequency shift can be related to particle mobility using the following equation:

.

FIG. 11A shows mobility data for determining the Zeta potential for the dispersion of carbon material obtained according to this example, and FIG. 11B shows a table summarizing data and characterization conditions. The zeta potential is defined as -63.93 mV for dispersion.

EXAMPLE 5B

In this example, graphene-containing carbon material is produced by shearing according to embodiments of the methods described herein.

Propane is used as the delivered gaseous organic compound, mineral oil is used as the liquid organic compound, and a battery shift reactor is used. FIG. 12A shows an SEM image of a micron graphene wafer obtained according to this example. The EDS data in FIG. 12B and those shown below in Table 3 summarize the atomic fractions of the elements.

Table 3

Spectrum Label Concentration
C (% atom) Concentration
O (% atom) Total
Concentration (% atom) Spectrum 69 99.51 0.49 100.00

The carbon material showed an oxygen concentration of 0.49% atom.

EXAMPLE 5C

In this example, graphene-containing carbon material is produced by shearing according to embodiments of the methods described herein.

A stack reactor with a shift is used, such as in FIG. 19. In this example, a variety of combinations of a gaseous organic compound and a liquid organic compound are used to produce a carbonaceous material: (i) propane and mineral oil, (ii) propane and toluene, and (iii) acetylene and toluene, respectively. Crystalline graphene is obtained in option (i) and micron graphite material is obtained in options (ii) and (iii).

EXAMPLE 6

In this example, a carbon material including graphene is produced using ultrasonic cavitation according to embodiments of the methods described herein. Use a cavitation reactor with an ultrasonic probe, using lever No. 8 and 90% power. The method is carried out for 15 minutes. The injection rate of the gas or entrainment flow is optionally 14 l/min. The following combinations of gaseous organic compound and liquid organic compound are used: (i) propane and toluene; (ii) Propane/E30 and Mobile-1, where E30 means the propane was pre-captured in Mobil-1 at 30 psi. in a pressure tank; (iii) propane/B and toluene meaning propane is "sparged"; and (iv) acetylene/B and toluene. "B" stands for "sparged". In option (i), (iii) and (iv), get micron graphene carbon material. In option (ii), a crystalline graphene material is obtained. Because everything was done at high shear, shear breaks the micron graphene-like slabs into crystalline (less than 10 nm) particles.

EXAMPLE 7

In this example, a carbon material including graphene is produced using a multifunctional cavitation reactor, according to embodiments of the methods described herein, including hydrodynamic cavitation and shear. Propane is used as the gaseous organic compound, and mineral oil is used as the liquid organic compound. A crystalline carbon material was formed.

EXAMPLE 8

This example demonstrates that the carbon material is not formed in the absence of a gaseous organic compound under otherwise equivalent process conditions for producing a solid carbon material.

Solid carbon material such as graphene is produced using a shift stack reactor using propane as the gaseous organic compound and Syn 530 as the liquid organic compound. Under equivalent conditions, without delivering a gaseous organic compound, the process does not produce a solid carbon material. Dispersing the resulting carbon material in Syn 530 results in a 14.6% reduction in wear scar and a 64.5% reduction in coefficient of friction relative to Syn 530 containing no carbon material.

Solid carbon material such as graphene is produced using a shift stack reactor using propane as the gaseous organic compound and MOBILE 1™ as the liquid organic compound. Under equivalent conditions, without delivering a gaseous organic compound, the process does not produce a solid carbon material. Dispersion of the resulting carbon material in MOBILE 1™ results in an 8% reduction in wear marks and a 31% reduction in coefficient of friction relative to MOBILE 1™ containing no carbon material.

EXAMPLE 9

In this example, a carbon material including graphene is produced using shear, according to embodiments of the methods described herein. Propane is used as a gaseous organic compound. A variety of organic liquids are used in combination with propane: Syn 530, MOBILE 1™, AMSOIL™, NonSyn, QUAKER STATE™ 530 and High Carbon Oil (HCO)/Base Oil.

Also in this example, friction reduction is demonstrated using a dispersion of carbon material in the organic fluids listed above. In the case of Syn 530 (see FIG. 14), a wear scar reduction of 14.6% and a friction coefficient reduction of 64.5% were demonstrated relative to Syn 530 without carbon material (i.e. relative to Syn 530 not used in method for producing hard carbon material according to this example). In the case of MOBILE 1™ (see FIG. 16), an 8% reduction in wear footprint and a 31% reduction in coefficient of friction was demonstrated relative to MOBILE 1™ not containing carbon material (i.e. relative to MOBILE 1™ not used in the hardening process). carbon material according to this example). In the case of AMSOIL™ (see FIG. 15), a 0% reduction in wear footprint and a 12% reduction in coefficient of friction was demonstrated relative to AMSOIL™ not containing hard carbon material (i.e. relative to AMSOIL™ not used in the hard carbon material process). according to this example). NonSyn, Quaker 530 demonstrated a 3% reduction in wear scar and a 19% reduction in coefficient of friction relative to NonSyn, Quaker containing no carbon material (i.e., relative to NonSyn, Quaker not used in the hard carbon material production process according to this example). In the case of HCO/Base oil, a 7% reduction in wear scar and a 13% reduction in friction coefficient relative to HCO/Base oil without carbon material (i.e. relative to HCO/Base oil not used in the hard carbon material production method according to this example).

EXAMPLE 10

In this example, a carbon material including graphene is produced using shear, according to embodiments of the methods described herein. Propane is used as the gaseous organic compound, and carbon disulfide is used as the liquid organic compound. FIG. 13A shows an SEM image of a carbon material formed according to the method of this example. FIG. 13A is labeled with box #78 and box #79. FIG. 13B shows EDS data corresponding to the material in box 78 (Spectrum 78) and box 79 (Spectrum 79). Table 4 summarizes the atomic fractions of the elements.

Table 4

Concentration (% atom) Spectrum Label C O Na mg Si S Fe Cu Zn Br sn Total Spectrum 78 90.09 7.29 0.23 0.03 0.50 1.33 0.27 0.23 0.03 100.00 Spectrum 79 47.67 4.42 0.58 15.25 1.50 27.85 2.10 0.63 100.00

As can be seen from Table 3, the formed carbon material contains a carbon-sulfur composite material in square 79. The compound has approximately 48% atom. carbon and 15% atom. sulfur.

EXAMPLE 11A

In this example, a graphene-incorporating carbon material is prepared using ultra-high shear using a Ross Model HSM-703X-20 Inline High Shear Mixer, according to embodiments of the methods described herein, such as the shear reactor of FIG. 18. Propane is used as the gaseous organic compound and mineral oil is used as the liquid organic compound. A gas injection pressure of 50 psi was used, the shift reactor was started at 10,000 rpm, and the synthesis process was carried out for 15 minutes.

The mineral oil carbon dispersion obtained in this example is characterized by a Zeta potential of -51 mV (eg -50.68 mV) as shown in FIG. 17A-17B.

The following description of characterization methods and conditions applies to Example 11A and Example 11B:

Test Equipment: Zeta Potential Analyzer, DELSA™ Nano C Nanoparticle Size and Zeta Potential Analyzer (Beckman Coulter, Brea, CA). DELSA™Nano C uses photon correlation spectroscopy (PCS) and electrophoretic light scattering techniques to determine particle size and Zeta potential of materials. Offering an excellent degree of accuracy, resolution and reproducibility, the DELSA™ Nano C is designed to simplify submicron particle and Zeta potential analysis. DELSA™Nano C provides accurate size measurement in the range of 0.6 nm to 7 µm at sample concentrations from 0.001% to 40%. It can analyze aqueous and non-aqueous samples, as well as determine the Zeta potentials of solid surfaces and membranes. It serves in a variety of industrial applications such as nanotechnology, electronics, pharmaceuticals, inks, food & beverage, biomedicine, textiles.

, где D является константой диффузии, k_B является константой Больцмана, T является абсолютной температурой, ƞ₀ является вязкостью и d является диаметром сферической частицы.Particles suspended in liquids are in Brownian motion due to random collisions with solvent molecules. This movement causes the particles to diffuse through the medium. The diffusion coefficient, D, is inversely proportional to particle size according to the Stokes-Einstein equation:

, where D is the diffusion constant, k _B is the Boltzmann constant, T is the absolute temperature, ƞ ₀ is the viscosity, and d is the diameter of the spherical particle.

Photon correlation spectroscopy, sometimes also called dynamic light scattering, is a technique used to determine the diffusion coefficient of small particles in a liquid. The coefficient is determined by accurately measuring the light scattering intensity of the particles as a function of time. As the particles of interest diffuse through the sample cell due to Brownian motion, the incident laser light beam irradiates the particles. Particles scatter light, producing fluctuations in scattering intensity as a function of time. Scattered light is collected at a selected angle and measured with a highly sensitive sensor. Since the rate of diffusion of particles is determined by their size, information about their size is contained in the rate of oscillation of light scattering. The intensity fluctuations are collected as photon pulses and correlated to create an autocorrelation function (ACF). The diffusion coefficient is determined by fitting the ACF using the Cumulants method, from which the average size is obtained using the Stokes-Einstein equation.

The zeta potential is a measure of the electric potential in the glide plane in the double layer surrounding a particle suspended in solution. The double layer consists of a Stern layer and a diffuse layer. In the Stern layer, ions with the opposite charge of surface particles are attracted to the particle. As the distance from the particle surface increases, oppositely charged ions become more diffuse. The point where the ions begin to diffuse into the environment is called the slip plane, since the strongly attracted ions will move with the particle in Brownian motion. The zeta potential is measured on the glide plane. The zeta potential can be used as a measure of the stability of a particle in solution. Particles with a Zeta potential greater than +/-20 mV are considered stable because the charge keeps the particles from agglomerating. Conversely, particles with a Zeta potential closer to 0 mV tend to collide and form large agglomerates.

Electrophoretic light scattering is a technique used to determine the Zeta potential of charged particles in solution. The slip plane charge cannot be measured directly on the DELSA™ Nano C analyzer. Instead, the Zeta potential is determined through theoretical models and electrophoretic mobility. An electric field is applied to particles in solution. The particles will move towards the oppositely charged electrode. The particles are irradiated with laser light and scattered due to particle motion. The detected scattered light creates a frequency shift from the incident laser beam. The frequency shift can be related to particle mobility using the following equation:

, где D является частотой сдвига частиц, U является подвижностью частиц, q является вектором рассеивание, λ является длиной волны падающего света, n является показателем преломления среды, и θ является углом рассеивания. Зная подвижность, уравнение Смолучовски можно применить для того, чтобы найти Дзета-потенциал.

, где ε0 и εr являются диэлектрическими константами в вакууме и среде, соответственно.

, where D is the particle shear frequency, U is the particle mobility, q is the scattering vector, λ is the wavelength of the incident light, n is the refractive index of the medium, and θ is the scattering angle. Knowing the mobility, the Smoluchowski equation can be applied to find the Zeta potential.

, where ε0 and εr are the dielectric constants in vacuum and medium, respectively.

In addition to measuring the Zeta potential of particles in solution, the Zeta potential of a solid surface can also be determined. The same principles used to measure the Zeta potential of a particle apply to a flat surface. A specially designed Flat Surface Cell is used to hold solid samples. The procedure for measuring the Zeta potential of a solid surface is similar to the typical measurement of the Zeta potential for particles. Measurements are carried out using dynamic light scattering of charged test particles under the influence of both electroosmosis and electrophoresis. The true electroosmotic flow due to the Zeta potential of the solid surface is obtained by subtracting the true electrophoretic mobility from the total apparent electroosmotic flow of charged test particles.

Test Conditions and Parameters: Prior to Zeta potential analysis, the sample is mixed and about 5 ml of the sample is centrifuged at 3000 rpm for 20 minutes. ~1 ml aliquot is taken from the top of the centrifuged sample and used for analysis. To determine the Zeta potential, the sample is analyzed with a Flow Cell using electrophoretic light scattering. Reference values from the literature 1.467 for the refractive index of the diluting oil [Ref. 1], 19.1 cP for dilution oil viscosity [Ref. 2], and 2.1 for the dielectric constant of oil [Ref. 3], they use experimental data for analysis and calculation of the Zeta potential. Table 5 summarizes the test conditions and test parameters.

Table 5 Zeta Potential Test Conditions and Parameters

Sample One sample of light mineral oil with graphene oil sample of light mineral with graphene Test instrument DELSA™ Nano C Methodology Electrophoretic light scattering Dimension cell flow cell Refractive index of diluent 1.467 Thinner viscosity 19.1 cP Dielectric constant of diluent 2.1 Test temperature 25°C Room temperature 22.8°C (73°F) Humidity 40% RH

Links for examples 11A and 11B:

1. Millipore Sigma (2019). Liquid Refractive Index-Mineral Oil. https://www.sigmaaldrich.com/catalog/product/sial/nist1922?lang=en&region=US

2. EFSA Panel on Food Additives and Nutrient Sources added to Food (ANS); Scientific Opinion on the use of high viscosity white mineral oils as a food additive on request from the European Commission. EFSA Journal , 2009;7(11):1387.

3 Honeywell (2019). Dielectric Constant Table. www.honeywellprocess.com

EXAMPLE 11B

In this example, a carbon material including graphene is produced using shear, according to embodiments of the methods described herein, such as the shear reactor of FIG. 18. Propane is used as the gaseous organic compound and MOBILE 1™ oil is used as the liquid organic compound. A gas injection pressure of 30 psi was used, the shift reactor was started at 12,000 rpm, and the synthesis process was carried out for 15 minutes.

The carbon dispersion in MOBILE 1™ obtained in this example is characterized by a Zeta potential of -64 mV (eg -63.93 mV).

EXAMPLE 12A

This example describes mechanically stirred reactors, which can also be described as high temperature, high pressure reactors (SHTHPTR). FIG. 23 illustrates a typical mechanically stirred reactor that is compatible with the methods described herein, in accordance with certain embodiments. Stirred reactor or SHTHPTR, of FIG. 23 facilitates gas-liquid mass transfer between a carbon-based gas and a carbon-based liquid to create a chemical reaction that can produce graphene or a graphene-like material, functionalize a graphene material, or facilitate the creation of a graphene-like composite material. In this reactor, the synthesis gas is dispersed into small bubbles to dissolve in the liquid. Smaller bubbles have a larger surface area and thus facilitate gas-liquid mass transfer.

Stirred reactors, which can be used in the same way as gas-liquid mass transfer reactors according to the embodiments described herein, include mechanically stirred reactors, which can be divided into turbine, monolithic or foam reactors.

Generally, the low solubility of the organic gas in the carbon liquid can be improved by the operation of a reactor such as the mechanically agitated gas-liquid mass transfer reactor of FIG. 23 at elevated pressures, for example, from 6 bar (about 87 psi) to 150 bar (about 2175 psi). The operating temperature of the reactor is typically in the range of 20°C to 250°C (e.g. 20°C to 200°C, 20°C to 150°C, 20°C to 100°C, 30°C to C to 250°C, 30°C to 200°C, 30°C to 150°C, 30°C to 100°C, 40°C to 250°C, 40°C to 200°C , 40°C to 150°C, 40°C to 100°C, 50°C to 250°C, 50°C to 200°C, 50°C to 150°C, 50°C up to 100°C, 50°C to 90°C or 60°C to 100°C).

A gas-liquid mass transfer reactor with mechanical agitation, such as in FIG. 23 contains a stirrer. Without wishing to be bound by any theory, it is believed that organic gas-organic liquid reactions have limited mass transfer. Thus, the agitation system is important to: (1) enhance mass/liquid exchange, (2) enhance heat transfer to speed up the chemical reaction, and (3) homogenize the gas/liquid mixture to prevent uneven temperature and concentration profiles during the reaction process. The agitator is an important component of a high temperature, high pressure mechanically agitated reactor, and can be of several types, including but not limited to: Rushton agitator/turbine, monolithic agitator, helical agitator, radial plate agitator, flat impeller, axion propeller, angled blades, turbine vortex mixer, several mixers on one rod.

Preferably, but not necessarily, the agitator used to increase gas-liquid mass transfer is a gas-inducing agitator such as shown in FIG. 24. This highly efficient impeller disperses the carbon gas in the upper space of the reactor into very fine gas bubbles and thus creates an extremely large gas-liquid interface.

The gas-inducing impeller used in this example comprises a hollow stainless steel impeller shaft with a small 1mm gas inlet at the top of the impeller shaft in the upper space of the mixing vessel. The gas in the upper space is sucked into the body of the lionfish and then dispersed into the liquid phase through the gas dispersion ports (exit) in the lionfish located at the end of each of the 4 blades of the lionfish. This impeller is installed in the SHTHPTR (FIG. 23) with an electric or pneumatic agitator to provide continuous rotation for long runs. The higher the stirring speed, the higher the vacuum and the higher the driving force. For maximum suction through the gas ports, the lionfish can typically be operated in the 100-3000 rpm range (eg 600-2000 rpm, 1000-1200 rpm, 100-600 rpm). Lionfish can be purchased from any suitable supplier such as Parr Instrument Company (Moline, IL).

EXAMPLE 12B

In this example, a graphene-like material is produced and characterized using a mechanically stirred reactor such as in FIG. 23. FIG. 25 shows an SEM showing a graphene-like material with few layers produced in a high temperature, high pressure mechanically stirred reactor (e.g., FIG. 23) via injecting propane gas into liquid toluene for 30 minutes at 80 psi. and temperature 60°C. The resulting solid carbon material is a graphene-like material (FIG. 25) rather than amorphous carbon.

Process vessel parameters for this example include: a 9" (22.86 cm) diameter vessel containing 2 liters of toluene and a 4" (10.16 cm) impeller rotating at 3000 rpm for 30 minutes. The ratio of impeller diameter to reservoir diameter (D/T) is 0.44. The shear created by the impeller in a stirred reactor is mainly determined by the ratio of impeller diameter to vessel diameter (D/T). For the process of the invention, the D/T ratio is generally in the range of 0.1 to 0.6, preferably 0.2 to 0.5. Low D/T impellers can produce high shear at lower rpm, while high D/T configurations tend to operate at higher rpm and cause low shear but more mixing. In the process of the invention, it has been found that a low D/T ratio is desirable because the goal is not mixing, but rather maximizing gas transfer through high shear.

EXAMPLE 12C

In this example, a dispersion of a graphene-like material in a high-carbon oil without additives is made using a mechanically stirred reactor, such as the reactor of FIG. 23. In this example, the dispersion is used for lubrication and the lubrication properties are compared with those of the same oil without the graphene-like material. The high carbon oil is treated for 40 minutes with propane injection at 30 psi. at 60°C. Table 6 shows the improvement in lubrication using the resulting dispersion compared to oil to obtain a graphene-like material.

Table 6

Wear marks Friction coefficient Graphene free 1 0.115 With graphene in situ 0.84 0.101 % Improvement 19% 14%

EXAMPLE 13

This example demonstrates the reduction of graphene oxide (GO) to reduced graphene oxide (rGO), according to certain embodiments of the methods described herein.

A key topic in the research and applications of graphene oxide (GO) is the reduction of GO to reduced graphene oxide (rGO). The disadvantage of most of the processes used to convert GO to rGO is that the quality of the graphene is reduced. This is because lattice defects and functional groups attached to the surface and edges cannot be completely removed during the redox step. Also a problem is that the strong oxidizers, liquid wastes and organic solvents used in the recovery process raise environmental issues. On the contrary, certain methods described herein are much simpler and do not compromise the quality of graphene or do not require environmentally hazardous chemicals.

FIG. 26-27 show the reduction of GO to rGO using battery shift to sparge propane into GO dispersed in the polar solvent N -methyl-2-pyrrolidone (NMP). This process results in a reduction in atomic oxygen in GO from 34% to 20%, which increases the C/O ratio from 1.76 to 3.81. The carbon added to GO comes from additional carbon created during the gas-liquid mass transfer process. FIG. 26 and Table 7 summarize the atomic fractions of elements in graphene oxide.

Table 7

Concentration (% atom) Spectrum label C O Na Si Cl K Total 2 293 GO 1550x region 1 64.18 34.74 0.17 0.12 0.67 0.12 100.00 2 293 GO 1500x region 2 64.51 34.39 0.17 0.13 0.66 0.13 100.00

FIG. 27 and Table 8 summarize the atomic fractions of elements in reduced graphene oxide (reduced graphene oxide of FIG. 26).

Table 8

Concentration (% atom) Spectrum Label C O mg Si S Cl Ca Cu Zn Pb Total Region 1 74.05 20.78 0.32 0.33 0.15 0.19 2.61 0.61 0.40 0.56 100.00 Region 2 74.83 19.59 0.35 0.41 0.11 0.21 2.81 0.67 0.35 0.66 100.00

EXAMPLE 14A

In this example, graphene has an oxidized edge as an example of in situ functionalization of graphene, according to certain embodiments described herein.

Edge-oxidized graphene is the antithesis of graphene reduction. Instead of removing oxygen, it is legally added. The main reason for adding oxygen to pure graphene is to make the graphene water-dispersible. This is not an easy task because high quality graphene has very few defects that make graphene hydrophobic. The dilemma is that for graphene to be dispersed in water, it must have defective sites. At present, the most common way to obtain aqueous graphene dispersions with low oxygen content is to graft several chemical groups onto limited defect sites on pure graphene.

This example demonstrates the environmentally friendly process of mild oxidation of high quality graphene. Gas-liquid mass transfer reactors can be used to obtain "weak" oxidation of graphene in a way that avoids significant damage to the lattice of graphene plates. Minimal damage is provided by graphene, which is soluble in water without any surfactants or additives. Oxygen bubbling with sonication also lowers the surface tension of water to about 42, which is close to matching the surface tension of graphite. Those skilled in the art will recognize that liquid separation is facilitated when the surface tension of the liquid is close to the surface tension of the graphite. However, the use of oxygen sparging to lower the surface tension of water for liquid separation is not reported. This process does not require the use of surfactants, water/alcohol mixtures or expensive, environmentally hazardous solvents. The idea of oxygen saturation lowering the surface tension of water is supported by recent molecular dynamics modeling (see, for example, Jain, et al., AIP Advances , 2017, 7, 045001).

EDS analysis in FIG. 28-29 shows that after 1 hour of treatment of pure graphene with oxygen injected into the hydrodynamic cavitation reactor, the oxygen on the graphene rises from ~0.5% to ~6% and the graphene becomes water soluble. FIG. 28 and Table 9 summarize the atomic fractions of elements in pure graphene.

Table 9

Concentration (% atom) Spectrum label C O Total Spectrum 5 99.43 0.57 100.00 Spectrum 6 99.60 0.40 100.00

FIG. 29 and Table 10 summarize the atomic fractions of elements in partially oxidized (oxidized edge) graphene (oxidized graphene of FIG. 28).

Table 10

Concentration (% atom) Spectrum label C O F Na S Cl Cu Total Spectrum 80 92.14 5.96 0.39 0.14 1.24 0.06 0.08 100.00

EXAMPLE 14B

In this example, the oxidized edge graphene from Example 14A is used to improve the lubricity of water-based lubricants. More specifically, in FIG. 30 shows that when water-dispersed graphene is added to the aqueous portion of Master Chemical 685, there is a 26% recovery in the torque required to form filaments in the steel. The top graph is graphene-free coolant and the bottom graph is 0.01% edge-oxidized graphene. Lower torque reflects higher lubricity.

EXAMPLE 15

In this example, cationic graphene (CGN) is produced according to certain embodiments described herein. The choice of electrical properties of graphene through the creation of cationic graphene is of great importance in a wide area of modern electronic devices. Chemical doping is an important approach to choosing the electronic property of graphene. Generally, there are two ways of chemical doping of graphene: (1) adsorption of metal or organic molecules on the surface of graphene, or (2) replacement doping, which introduces heteroatoms such as nitrogen atoms and boron atoms into the carbon lattice of graphene. Both of these methods can change the electronic properties of graphene.

This example shows another way to change the electronic nature of graphene. Although graphene is usually anionic, the gas-liquid mass transfer process can be used to produce cationic graphene in situ. The process includes, for example, sparging propane into 1,2-dichlorobenzene with high shear. Under these conditions, the gas-liquid mass transfer reaction converts carbon in the gas/liquid system with high shear into graphene in situ. Cationic graphene produced from 1,2-dichlorobenzene using the gas-liquid mass transfer described herein has a Zeta potential of +4.99 mV as seen in FIG. 31. This is different from the -33 mV zeta potential for graphene dispersed in N-methyl-2-pyrrolidone (NMP).

STATEMENTS REGARDING INTRODUCTION AS A REFERENCE AND VARIATIONS

All references, including publications, patent applications, and patents cited herein, are hereby incorporated by reference to the same extent as if each reference were individually and specifically indicated as being incorporated by reference and were set forth herein as a whole.

The use of the terms "a" and "an" and "the" and "at least one" and similar objects of reference in the context of the description of the invention (especially in the context of the following claims) is to be construed as embracing singular and plural, unless otherwise indicated. otherwise in this document, or is clearly inconsistent with the context. The use of the term "at least one" followed by a list of one or more items (e.g. "at least one of A and B") should be construed to mean one item selected from the listed items (A or B ) or any combination of two or more of the listed items (A and B), unless otherwise specified in this document, or is clearly inconsistent with the context. The terms "including", "having", "includes" and "comprising" are to be construed as open terms ( i.e. , meaning "including but not limited to") unless otherwise noted. The listing of value ranges in this document is simply intended to serve as a shorthand way of referring separately to each individual value falling within the range, unless otherwise noted herein, and each individual value is included in the specification as if it were individually listed. in this document. All of the methods described herein may be performed in any suitable order unless otherwise indicated herein or clearly contradicted by the context. The use of any and all examples or exemplary language (eg, "such as") provided herein is intended only to better illuminate the invention and does not limit the scope of the invention unless otherwise stated. No language in the specification is to be construed as indicating an unclaimed element as essential to the practice of the invention.

When the Markush group or another group is used herein, all individual members of the group and all combinations and subcombinations possible within the group are intended to be individually included in the description. If a compound described herein, such as a specific isomer, enantiomer, or diastereomer of a compound, is not defined, such as in a formula or chemical name, then the description is intended to include each isomer and enantiomer of the compound described alone or in any combination. In addition, unless otherwise indicated, all isotopic variants of the compounds described in this document are covered by the description. For example, it will be understood that any one or more hydrogen atoms in the described molecule can be replaced by deuterium or tritium. Isotopic variants of a molecule are commonly used as standards in analyzes of the molecule and in chemical and biological studies related to the molecule or its use. Methods for producing such isotopic variants are known in the art. The specific names of the compounds are exemplary, since it is known that a person skilled in the art may name the same compounds differently.

Certain molecules described herein may contain one or more ionizable groups (groups from which a proton may be removed (eg, -COOH) or added (eg, amines) or which may be quaternized (eg, amines)). All possible ionic forms of such molecules and their salts are included individually in the description of this document. With respect to the salts of the compounds herein, one of skill in the art can select from among the wide variety of available counterions those suitable for the preparation of the salts of the present invention for a given application. In certain applications, the choice of a given anion or cation to form a salt may result in an increase or decrease in the solubility of that salt.

Each method and system described or exemplified herein can be used to practice the invention unless otherwise indicated.

Preferred embodiments of this invention are described herein, including the best method known to the inventors for carrying out the invention. Changes to the preferred embodiments may become apparent to those skilled in the art upon reading the above description. The inventors expect those skilled in the art to make appropriate use of such modifications, and the inventors contemplate that the invention may be practiced otherwise than as specifically described herein. Accordingly, this invention includes all modifications and equivalents of the subject matter set forth in the claims appended to this document, as permitted by applicable law. In addition, any combination of the above elements in all possible variations is covered by the invention, unless otherwise indicated in this document, or clearly does not contradict the context.

Claims (55)

1. A method for producing a solid carbon material, including: delivering a liquid containing at least one liquid organic compound to the reaction zone of the reactor; delivering a gas containing at least one gaseous organic compound to the reaction zone of the reactor; And inducing a chemical reaction involving gas-liquid mass transfer between at least one liquid organic compound and at least one gaseous organic compound, wherein: the chemical reaction takes place in the reaction zone of the reactor; solid carbon material obtained by the reaction; the solid carbon material is obtained during the reaction in the form of a dispersion comprising the solid carbon material dispersed in a liquid; the chemical reaction is a homogeneous reaction including homogeneous nucleation of solid carbon material in the reaction zone of the reactor; no chemical reaction takes place on or in the catalyst; And the resulting solid carbon material is selected from the group consisting of graphite , expanded graphite, graphite-like material, graphene, graphene-like material, carbon slabs, carbon nanotubes, carbon onions, other carbon allotrope, graphene-containing composite, cationic graphene, or any combination thereof. 2. The method of claim 1 wherein the composition of the gas is different from the composition of the liquid. 3. The method of claim 1, wherein the composition of the at least one gaseous compound is different from the composition of the at least one liquid organic compound. 4. The method of claim 1, wherein the method does not include heterogeneous nucleation of a solid carbon material on a solid support. 5. The method according to p. 1, in which the stage of delivering liquid is performed through the first input stream to the reaction zone and the step of delivering gas is performed through the second input stream to the reaction zone; however, the paths of the first stream and the second input stream are different and are physically separate. 6. The method of claim 1, wherein the liquid delivery step and the gas delivery step are performed simultaneously or the gas delivery step is performed after the liquid is delivered to the reaction zone. 7. The method of claim 1 wherein the solid carbon material remains dispersed in the liquid while in the reaction zone. 8. The method of claim 1, wherein the liquid does not contain solid carbon material during the liquid delivery stage and prior to the gas delivery and chemical reaction induction stages. 9. The method of claim 1, wherein the liquid is free of solids and is not a colloid, suspension, or sol during the liquid delivery step and up to the gas delivery and chemical reaction induction steps. 10. The method of claim 1 wherein the solid carbon material is only formed in the reaction zone of the reactor. 11. The method of claim 1 wherein no solid carbon material is produced if the method is performed without a gas delivery step. 12. The method of claim. 1, in which the delivery of gas includes capturing gas in liquid, injecting gas into liquid, sparging gas into liquid, or a combination of both. 13. The method of claim 1 wherein the gas is delivered directly to the reaction zone during the gas delivery step. 14. The method of claim 1 wherein the step of inducing a chemical reaction comprises inducing a shear force in the fluid. 15. The method of claim 1, wherein the step of inducing a chemical reaction comprises agitating or mixing a liquid and a gas in the reaction zone, optionally under pressure. 16. The method according to claim 1, in which: the reactor is a cavitation reactor; the reaction zone is the cavitation zone of the cavitation reactor; And the method includes the formation of cavitation bubbles in the liquid in the cavitation zone of the cavitation reactor. 17. The method of claim 16, wherein during the gas delivery step, the gas is delivered directly to or within 1 mm of the cavitation bubble nucleation region, the cavitation bubble nucleation region corresponding to the cavitation bubble nucleation in the hydrodynamic cavitation reaction during the formation step. 18. The method of claim 16, wherein the step of forming includes forming a cavitation cloud containing cavitation bubbles in the cavitation zone of the reactor, wherein the gas is delivered directly into or within 1 mm of the cavitation cloud. 19. The method according to p. 16, in which the stage of formation includes the formation of a cavitation cloud containing cavitation bubbles; in this case, the carbon material is formed in a cavitation cloud. 20. The method of claim 16, wherein the liquid does not contain carbon material during the liquid delivery step and prior to the formation of cavitation bubbles. 21. The method of claim 16, wherein the cavitation reactor comprises a hydrodynamic cavitation reactor having a pre-cavitation zone and an orifice zone, wherein the orifice zone is located between the pre-cavitation zone and the cavitation zone; the hole zone includes at least one hole, while the liquid flows from the pre-cavitation zone to the cavitation zone through at least one hole; wherein each of the at least one orifice is characterized by an orifice diameter that is smaller than the diameter of the pre-cavitation zone. 22. The method according to p. 21, in which the gas is delivered directly to the cavitation end of at least one hole or within 1 mm from the end of at least one hole; moreover, the cavitation end of at least one hole is the end of at least one hole closest to the cavitation zone of the cavitation reactor. 23. The method of claim 1, wherein the gaseous organic compound is selected from the group consisting of alkane, alkene, alkyne, cycloalkane, heterocycloalkane, arene, heteroarene, and combinations thereof, wherein the alkane, alkene, alkyne, cycloalkane, heterocycloalkane, arene, or heteroarene may optionally be substituted with one or more substituents. 24. The method of claim 1, wherein the at least one gaseous organic compound is selected from the group consisting of methane, acetylene, ethylene, propane, 1,3-butadiene, butane, and any combination thereof. 25. The method of claim 1, wherein the at least one liquid organic compound is selected from the group consisting of a monomer, an oligomer, a prepolymer, a polymer, an organic solvent, and any combination thereof. 26. The method according to any one of paragraphs. 1-13, in which at least one liquid organic compound is selected from the group consisting of methanol, ethanol, isopropyl alcohol, methylpyrrolidone, d-cyclopentadiene, hexane, benzene, toluene, heptane, xylene, dimethyl sulfoxide, mineral oil, machine oil, , base oil, hydrogenated castor oil, gear oil, gear oil, vegetable oil, hydrocarbon base drilling fluid, oil with additives, oil without additives, kerosene, diesel fuel, ethylene glycol, propylene glycol, diethylene glycol, triethylamine, trimethylamine, pentane, cyclopentane, cyclohexane , 1,4-dioxane, chloroform, diethyl ether, dichloromethane, tetrahydrofuran, ethyl acetate, acetone, dimethylformamide, acetonitrile, nitromethane, propylene carbonate, formic acid, butanol, propanol, acetic acid, octadecene, oleic acid, oleylamine, octane, diethylene glycol ether , 1,2-dichlorobenzene, methyl acetate, tetrachlorethylene, diphenylthiourea s, hexafluoro-2-propanol, cinnamic acid, trimethylamine, benzenethiol, ethanethiol, ethanedithiol, 4-aminobenzenethiol, acrylic acid, carbon disulfide, 1,2-dichlorobenzene, N-methyl-2-pyrrolidone, and any combination thereof. 27. The method of claim 1 wherein the liquid comprises water. 28. The method of claim 1 wherein the carbon material comprises graphene or a graphene-like material. 29. The method of claim 1 wherein the carbon material comprises a graphene polymer nanocomposite. 30. The method of claim. 1, in which the carbon material has an oxygen content of 7 at.% or less. 31. A solid carbon material dispersion obtained by the method of claim 1, characterized by a coefficient of friction reduced by at least 5% relative to the same liquid without the solid carbon material. 32. The use of a solid carbon material obtained by the method of claim 1 as part of a battery anode, battery cathode, conductive material, heat conductive material, lubricating fluid or heat conductive fluid. 33. Use of the dispersion obtained by the method of claim 1 to obtain a portion of a battery anode, battery cathode, conductive material, heat conductive material, lubricating fluid or heat conductive fluid. 34. The method of claim 1 further comprising functionalizing the solid carbon material to provide a functionalized solid carbon material. 35. The method of claim 1, wherein the dispersion is the first dispersion, the chemical reaction is the first chemical reaction, the solid carbon material is the precursor material, the gas is the first gas, and the reactor is the first reactor; wherein the method further comprises: delivering the first dispersion to the second reactor; delivering a second gas containing at least one gaseous organic compound directly to the reaction zone of the second reactor; And inducing a second chemical reaction in the reaction zone of the second reactor; and: the second chemical reaction converts the precursor material into a second solid carbon material; the second carbon material is dispersed in the liquid; And the precursor material and the second carbon material are different. 36. The method of claim 35, wherein the second reactor is a cavitation reactor and the induction step comprises forming cavitation bubbles in the first dispersion in the reaction zone of the second reactor. 37. The method of claim 35, wherein the first reactor and the second reactor are the same.

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