CN115404496A - Method for continuously preparing graphene oxide through two-step electrochemistry - Google Patents

Method for continuously preparing graphene oxide through two-step electrochemistry Download PDF

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CN115404496A
CN115404496A CN202211197331.XA CN202211197331A CN115404496A CN 115404496 A CN115404496 A CN 115404496A CN 202211197331 A CN202211197331 A CN 202211197331A CN 115404496 A CN115404496 A CN 115404496A
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anode
conveyor belt
graphite
graphene oxide
electrolyte
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韦覃伟
汪进华
黄坤
成会明
刘永生
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Shenzhen Matterene Technology Co ltd
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Abstract

The invention belongs to the field of preparation of graphene oxide materials, and particularly relates to a method for continuously preparing graphene oxide through two-step electrochemistry. Graphite with a macroscopic continuous structure is used as a raw material, the graphite raw material is limited and extruded by the space of a conveying device in the conveying process, a cathode and an anode are electrified under the condition of soaking in electrolyte, and the graphite raw material sequentially passes through an intercalation tank and an oxidation tank to respectively carry out intercalation reaction and oxidation reaction. In the electrochemical reaction, a graphite raw material is used as an anode, and anode substances after the oxidation reaction are stripped and cleaned to obtain the graphene oxide material. The method can ensure that the product is fully oxidized, the preparation process is continuous and efficient, and the method can be used for large-scale preparation of the graphene oxide material.

Description

Method for continuously preparing graphene oxide through two-step electrochemistry
Technical Field
The invention belongs to the field of preparation of graphene oxide materials, and particularly relates to a method for continuously preparing graphene oxide by a two-step electrochemical method.
Background
The graphene material has ultrahigh electrical conductivity, thermal conductivity and tensile strength, and has very wide application. Graphene oxide is an important derivative of graphene, and is generally used as a precursor for preparing a graphene material by reduction. Meanwhile, the surface of the graphene oxide contains a large number of oxygen-containing functional groups (such as hydroxyl, epoxy and carboxyl), so that the graphene oxide has good dispersibility and assemblability.
At present, a chemical oxidation method represented by a Hummers method is generally adopted for preparing graphene oxide in a large scale, and a strong oxidizing agent such as potassium permanganate is used for oxidizing a graphite raw material to prepare the graphene oxide. The research on the chemical oxidation method has never been stopped, but the problems of high pollution, easy explosion in the production process, huge water consumption and the like caused by the chemical oxidation method are not thoroughly solved all the time. The electrochemical oxidation method for preparing the graphene oxide adopts electrochemical oxidation to replace a highly-polluted strong oxidant, is an environment-friendly preparation method, and is considered to be the most promising preparation method capable of replacing the chemical oxidation method.
The common one-step electrochemical method is simple in reaction process, but the product generally has the problem of insufficient oxidation, and the oxidation level of graphene oxide prepared by the electrochemical method can be obviously improved by performing pre-intercalation treatment on the graphite raw material. Chinese patent publication No. CN 107215867A discloses a method for continuously preparing graphene oxide micro-sheets, which adopts a continuous graphite material as a reaction anode, and sequentially carries out intercalation reaction and oxidation exfoliation reaction to prepare graphene oxide. However, the strength of the intercalated graphite raw material is reduced, and a conductive path is easy to break in the transmission process, so that the intercalated graphite raw material is difficult to be applied to large-scale stable production. Therefore, a method for continuously, efficiently and stably preparing graphene oxide in a large scale through two-step electrochemical fermentation is needed.
Disclosure of Invention
Aiming at the defects of the prior art, the invention aims to provide a method for continuously preparing graphene oxide through two-step electrochemistry, which ensures that a reaction anode is stable and continuous in the conveying process and a conductive path is kept by carrying out space limitation and extrusion on a graphite raw material in the two-step electrochemical reaction processes of intercalation and oxidation, thereby realizing high-quality, continuous and stable electrochemical preparation of the graphene oxide.
The technical scheme of the invention is as follows:
a method for continuously preparing graphene oxide by two-step electrochemistry takes graphite with a macroscopic continuous structure as a raw material, the graphite raw material is used as an anode and is limited and extruded by a conveying device in the conveying process, a cathode and the anode are electrified under the condition of soaking in electrolyte, and the graphite raw material sequentially passes through an intercalation tank and an oxidation tank to respectively carry out intercalation reaction and oxidation reaction. In the electrochemical reaction, taking a graphite raw material as an anode, and stripping and cleaning an anode substance after the oxidation reaction is finished to obtain a graphene oxide material;
the device for realizing the method comprises an anode 1, a conductive roller 2, a power supply 3, a first guide roller 4, a second guide roller 5, a first conveyor belt 6, a second conveyor belt 7, a third guide roller 8, a conveyor belt buckle 9, an intercalation tank cathode group 10, an oxidation tank pole group 11, intercalation electrolyte 12 and oxidation electrolyte 13, and has the following specific structure: the anode 1 penetrates through the conductive roller 2 and enters between the first conveyor belt 6 and the second conveyor belt 7, the first conveyor belt 6 and the second conveyor belt 7 are respectively tightly attached to the upper surface and the lower surface of the anode 1, and the anode 1 is conveyed by the first conveyor belt 6 and the second conveyor belt 7 and sequentially passes through a filling layer of electrolyte 12 and an oxidizing electrolyte 13; the first conveyor belt 6 bypasses the first guide roller 4 and the third guide roller 8 and is closed on the upper surface of the anode 1; the second conveyor belt 7 bypasses the second guide roller 5 and the third guide roller 8 and is closed on the lower surface of the anode 1; when the first conveyor belt 6 and the second conveyor belt 7 on the lower surface of the anode 1 enter the intercalation electrolyte 12, the first conveyor belt 6 and the second conveyor belt 7 are sleeved with the conveyor belt buckle 9, so that the first conveyor belt 6 and the second conveyor belt 7 limit and extrude the space of the anode 1, and when the first conveyor belt 6 and the second conveyor belt 7 leave the oxidation electrolyte 13, the conveyor belt buckle 9 is taken down, and the pressure borne by the anode 1 is released; the conductive roller 2 is connected with the anode of the power supply 3 through a lead, the intercalation tank cathode group 10 and the oxidation tank cathode group 11 are connected with the cathode of the power supply 3 through leads, and the intercalation tank cathode group 10 and the oxidation tank cathode group 11 are respectively soaked in intercalation electrolyte 12 and oxidation electrolyte 13.
The method for continuously preparing the graphene oxide by two-step electrochemistry comprises the step of preparing a graphite raw material with a macroscopic continuous structure from one or two of natural graphite, artificial graphite, blocky graphite, crystalline flake graphite, aphanitic graphite, expanded graphite or graphite powderA sheet or a wire obtained from the above composite; the preferred graphite material has a density in the range of 1.0 to 2.0g/cm 3 The flexible graphite paper of (2).
In the method for continuously preparing graphene oxide through two-step electrochemistry, a conveying device comprises one or more combinations of a belt conveyor, a roller conveyor, a chain plate conveyor, a mesh belt conveyor or a suspension conveyor; the movement rate of the graphite raw material relative to the electrolyte is 0 to 100m/h, and the preferable range is 0.1cm/h to 50cm/h.
According to the method for continuously preparing the graphene oxide by the two-step electrochemistry, the pressure applied to the graphite raw material by the conveying device is constant or variable in the conveying process of the graphite raw material, and the pressure ranges of the graphite raw material in the intercalation reaction and the oxidation reaction are 0-50 MPa and 0-20 MPa respectively.
In the two-step electrochemical continuous preparation method of graphene oxide, the conveying device applies pressure to the graphite raw material in a manner including but not limited to one or more of limiting expansion space, spring fastening, electric pressurization, hydraulic pressurization or pneumatic pressurization.
According to the method for continuously preparing the graphene oxide by the two-step electrochemistry, the electrolytes in the intercalation tank and the oxidation tank are the same or different, and the electrolytes are selected from one or the mixture of more than two non-reaction systems of acid or salt; wherein the acid includes, but is not limited to, sulfuric acid, nitric acid, perchloric acid, phosphoric acid, hydrochloric acid, acetic acid, trifluoroacetic acid, trifluoromethanesulfonic acid, chlorosulfonic acid, or magic acid, and the salt includes, but is not limited to, ammonium sulfate, potassium sulfate, sodium sulfate, magnesium sulfate, potassium perchlorate, or sodium persulfate.
According to the method for continuously preparing the graphene oxide by the two-step electrochemistry, the electrolyte mass concentration range of the electrolyte in the intercalation tank is 0.01-100%, and the preferable range is 60-100%; the electrolyte mass concentration of the electrolyte in the oxidation tank is 0.01-100%, and the preferable range is 20-85%.
The method for continuously preparing the graphene oxide through two-step electrochemistry adopts the same or different cathode materials in the intercalation tank and the oxidation tank; cathode materials include, but are not limited to, platinum, copper, nickel, gold, or graphite corresponding plates, meshes, wires, or rods; the relative position of the anode and the cathode includes but is not limited to single cathode and single anode facing, two cathodes sandwiching one anode or cathode surrounding the anode, and the surface distance between the anode material and the cathode material is in the range of 0.1 mm-1 m.
According to the two-step electrochemical continuous preparation method of graphene oxide, the voltage applied between the anode and the cathode is continuous direct current voltage, pulse direct current voltage or alternating current voltage, the voltage range is 0.1-10 kV, and the preferable range is 1-100V.
According to the method for continuously preparing the graphene oxide by the two-step electrochemical method, the anode substance after the oxidation reaction is stripped in one or more modes of mechanical shearing, ultrasonic crushing, high-pressure homogenization and the like, and the anode substance after the oxidation reaction is cleaned in one or more modes of centrifugal cleaning, filter pressing cleaning, cross flow cleaning and the like.
The technical principle of the invention is as follows:
in the process of preparing graphene oxide by the two-step electrochemical method, a graphite raw material is used as a reaction anode, intercalation agent ions enter graphite interlayers under the action of an electric field in an intercalation reaction to form a first-order or low-order graphite interlayer compound, the strength of the intercalated graphite raw material is reduced due to the influence of intercalation and soaking, and in order to realize continuous and stable preparation of the two-step electrochemical method, the graphite raw material in the conveying process is subjected to space limitation and extrusion, so that the intercalated graphite raw material still keeps complete structure and a conductive path is not influenced, and the next oxidation reaction process can be carried out.
The graphite intercalation compound enters an oxidation tank to carry out oxidation reaction, the oxidant contains water molecules, and in the electrolysis process, free radical ions are generated in the water molecule decomposition process to oxidize the graphite intercalation compound to generate oxygen-containing functional groups. Meanwhile, oxygen produced by the anode in the electrolysis process enters the graphite layers, so that the interlayer spacing of the compound between the graphite layers is increased. By carrying out space limitation and extrusion on the graphite raw material, the graphite raw material can always keep a stable passage in the oxidation process, thereby realizing sufficient oxidation.
After the oxidation reaction is finished, the obtained graphene oxide block is easy to collect, the electrolyte cannot be polluted, and the graphene oxide block can be repeatedly used. And cleaning and stripping the collected graphene oxide blocks to obtain the single-layer graphene oxide material.
The invention has the advantages and beneficial effects that:
1. the electrolyte of the invention is not polluted, can be stably reused for a long time, has small electrolyte consumption, and the water consumption in the preparation process is less than 40 times of the product quality.
2. The preparation process of the invention does not introduce heavy metal ions, does not generate toxic and harmful gases, and has no pollution to the environment.
3. The preparation process is continuous and simple, and is easy for large-scale preparation.
4. The yield of the graphite oxide material prepared by the method is 140-160%, the monolayer rate of the obtained graphene oxide is more than 70%, and the carbon source molar ratio can reach 1.3.
Drawings
FIG. 1 is a schematic diagram of the structure and process of an apparatus used in the present invention;
FIG. 2 is a photograph of the microstructure of graphene oxide in example 1;
in the figure, 1-anode, 2-conductive roller, 3-power supply, 4-first guide roller, 5-second guide roller, 6-first conveyor belt, 7-second conveyor belt, 8-third guide roller, 9-conveyor belt buckle, 10-intercalation tank cathode group, 11-oxidation tank cathode group, 12-intercalation electrolyte and 13-oxidation electrolyte.
Detailed Description
The invention relates to a method for continuously preparing graphene oxide by two-step electrochemistry, which takes graphite with a macroscopic continuous structure as a raw material in the specific implementation process, wherein the graphite raw material is limited and extruded by a conveying device in the conveying process, a cathode and an anode are electrified under the condition of soaking in electrolyte, and the graphite raw material sequentially passes through an intercalation tank and an oxidation tank to respectively carry out intercalation reaction and oxidation reaction. In the electrochemical reaction, taking a graphite raw material as an anode, and stripping and cleaning an anode substance after the oxidation reaction is finished to obtain a graphene oxide material;
as shown in figure 1: the device for realizing the method comprises an anode 1, a conductive roller 2, a power supply 3, a first guide roller 4, a second guide roller 5, a first conveyor belt 6, a second conveyor belt 7, a third guide roller 8, a conveyor belt buckle 9, an intercalation tank cathode group 10, an oxidation tank pole group 11, intercalation electrolyte 12 and oxidation electrolyte 13, and has the following specific structure: the anode 1 penetrates through the conductive roller 2 and enters between the first conveyor belt 6 and the second conveyor belt 7, the first conveyor belt 6 and the second conveyor belt 7 are respectively tightly attached to the upper surface and the lower surface of the anode 1, and the anode 1 is conveyed by the first conveyor belt 6 and the second conveyor belt 7 and sequentially passes through a filling layer of electrolyte 12 and an oxidizing electrolyte 13; the first conveyor belt 6 is wound around the first guide roller 4 and the third guide roller 8 and is closed on the upper surface of the anode 1; the second conveyor belt 7 bypasses the second guide roller 5 and the third guide roller 8 and is closed on the lower surface of the anode 1; when the first conveyor belt 6 and the second conveyor belt 7 on the lower surface of the anode 1 enter the intercalation electrolyte 12, the first conveyor belt 6 and the second conveyor belt 7 are sleeved with the conveyor belt buckle 9, so that the first conveyor belt 6 and the second conveyor belt 7 limit and extrude the space of the anode 1, and when the first conveyor belt 6 and the second conveyor belt 7 leave the oxidation electrolyte 13, the conveyor belt buckle 9 is taken down, and the pressure borne by the anode 1 is released; the conductive roller 2 is connected with the anode of the power supply 3 through a lead, the intercalation slot cathode group 10 and the oxidation slot cathode group 11 are connected with the cathode of the power supply 3 through leads, and the intercalation slot cathode group 10 and the oxidation slot cathode group 11 are respectively soaked in the intercalation electrolyte 12 and the oxidation electrolyte 13.
The drawings and examples are intended to illustrate specific embodiments of the invention, and the following three examples are intended to illustrate the invention, but not to limit the scope of the invention.
Example 1.
In this embodiment, the anode 1 is graphite paper 1; the power supply 3 is a direct current power supply, the intercalation electrolyte 12 is concentrated sulfuric acid (98 wt%) 12, and the oxidation electrolyte 13 is dilute sulfuric acid (70 wt%) 13
The device used in the embodiment comprises graphite paper 1, a conductive roller 2, a direct current power supply 3, a first guide roller 4, a second guide roller 5, a first conveyor belt 6, a second conveyor belt 7, a third guide roller 8, a conveyor belt buckle 9, an intercalation tank cathode group 10, an oxidation tank cathode group 11, concentrated sulfuric acid (98 wt%) 12 and dilute sulfuric acid (70 wt%) 13. The concrete structure is as follows: graphite paper 1 passes through a conductive roller 2 and enters a space between a first conveyor belt 6 and a second conveyor belt 7, the first conveyor belt 6 and the second conveyor belt 7 are respectively tightly attached to the upper surface and the lower surface of the graphite paper 1, and the graphite paper 1 sequentially passes through concentrated sulfuric acid (98 wt%) 12 and dilute sulfuric acid (70 wt%) 13 under the transportation of the first conveyor belt 6 and the second conveyor belt 7. The first conveyor belt 6 bypasses the first guide roller 4 and the third guide roller 8 and is closed on the upper surface of the graphite paper 1; the second conveyor belt 7 bypasses the second guide roller 5 and the third guide roller 8 and is closed on the lower surface of the graphite paper 1. When the first conveyor belt 6 and the second conveyor belt 7 on the lower surface of the graphite paper 1 enter concentrated sulfuric acid (98 wt%) 12, two layers of the first conveyor belt 6 and the second conveyor belt 7 are sleeved with a conveyor belt buckle 9, so that the first conveyor belt 6 and the second conveyor belt 7 limit and extrude the graphite paper 1 in space; when the first conveyor belt 6 and the second conveyor belt 7 leave the dilute sulfuric acid (70 wt%) 13, the conveyor belt buckle 9 is removed, and the pressure on the graphite paper 1 is released. The conductive roller 2 is connected with the anode of the direct current power supply 3 through a lead, and the intercalation slot cathode group 10 and the oxidation slot cathode group 11 are connected with the cathode of the direct current power supply 3 through leads. The intercalation tank cathode assembly 10 and the oxidation tank cathode assembly 11 are immersed in concentrated sulfuric acid (98 wt%) 12 and dilute sulfuric acid (70 wt%) 13, respectively.
In this example, graphite paper with a thickness of 500 micrometers and a width of 50cm is used as a graphite raw material, graphite plates are used as reaction anodes to form cathode groups 10,11, two graphite plates of each cathode group are respectively positioned on two sides of the graphite paper in parallel, and the distance between the graphite plates and the surface of the graphite paper is 10cm. The DC power supply loads 5.0V voltage. The transport speed of the graphite paper relative to the electrolyte is 10cm/h. And collecting the anode substance after the oxidation reaction is finished, and carrying out shearing and filter pressing treatment to obtain the graphene oxide dispersion liquid. As shown in FIG. 2, the obtained graphene oxide has a monolayer rate of 80%, a sheet diameter distribution of 1-10 μm, a sheet thickness range of 0.5-10 nm, and a carbon-oxygen molar ratio of 1.5. The yield from graphite feedstock to graphene oxide dispersion was 150%.
Example 2.
At a density of 1.5g/cm 3 Carbon rope with diameter of 8mmFor the anode 1, 98% by mass of sulfuric acid is used as intercalation electrolyte 12, and 1M ammonium sulfate aqueous solution is used as oxidation electrolyte 13 to prepare graphene oxide, and other device structures are the same as those in example 1, and specific preparation parameters in this example are as follows:
and applying 10V direct current voltage between the cathode and the anode, providing a conveying speed of 20cm/h for the graphite raw material by using a conveying belt, collecting the anode material after the oxidation reaction is finished, and performing ultrasonic and centrifugal treatment to obtain the graphene oxide dispersion liquid. The obtained graphene oxide has a monolayer rate of 85%, the sheet diameter distribution of 1-10 microns, the sheet thickness range of 0.5-5 nm and the carbon-oxygen molar ratio of 1.5. The yield from graphite feedstock to graphene oxide dispersion was 140%.
Example 3.
At a density of 1.6g/cm 3 The method comprises the following steps of preparing graphene oxide by using a carbon cloth with the width of 40cm as an anode 1, using 95% sulfuric acid in mass fraction as an intercalation electrolyte 12, and using 50% sulfuric acid in mass fraction as an oxidation electrolyte 13, wherein the other device structures are the same as those in example 1, and the specific preparation parameters in this example are as follows:
a direct current voltage of 20V is applied between the cathode and the anode, and the conveying belt provides a conveying speed of 30cm/h of graphite raw materials. And collecting the anode substance after the oxidation reaction is finished, and carrying out ultrasonic treatment and centrifugal treatment to obtain the graphene oxide dispersion liquid. The obtained graphene oxide has a monolayer rate of 80%, a sheet diameter distribution of 1-20 micrometers, a sheet thickness range of 0.5-5 nanometers and a carbon-oxygen molar ratio of 2.0. The yield from graphite feedstock to graphene oxide dispersion was 130%.
The result shows that the continuous preparation of the graphene oxide can be realized, the product is fully oxidized, and the method is an efficient, green and low-cost large-scale preparation method of the graphene oxide and has great application value. The three examples above are further illustrative of the present invention, wherein several changes and modifications can be made to the transfer device and to the spatial constraints and manner of extrusion of the graphite feedstock without departing from the principles of the present technology and should be considered within the scope of the present invention.

Claims (10)

1. A method for continuously preparing graphene oxide through two-step electrochemistry is characterized in that graphite with a macroscopic continuous structure is used as a raw material, the graphite raw material is used as an anode and is limited and extruded by a conveying device in the conveying process, a cathode and the anode are electrified under the condition of soaking in electrolyte, the graphite raw material sequentially passes through an intercalation tank and an oxidation tank to respectively carry out intercalation reaction and oxidation reaction, and anode substances after the oxidation reaction are stripped and cleaned to obtain a graphene oxide material;
the device for realizing the method comprises an anode (1), a conductive roller (2), a power supply (3), a first guide roller (4), a second guide roller (5), a first conveying belt (6), a second conveying belt (7), a third guide roller (8), a conveying belt buckle (9), an intercalation tank cathode group (10), an oxidation tank pole group (11), intercalation electrolyte (12) and oxidation electrolyte (13), and the specific structure is as follows: the anode (1) penetrates through the conductive roller (2) and enters a position between the first conveyor belt (6) and the second conveyor belt (7), the first conveyor belt (6) and the second conveyor belt (7) are respectively tightly attached to the upper surface and the lower surface of the anode (1), and the anode (1) is conveyed by the first conveyor belt (6) and the second conveyor belt (7) and sequentially filled with the electrolyte (12) and the electrolyte (13); the first conveyor belt (6) bypasses the first guide roller (4) and the third guide roller (8) and is closed on the upper surface of the anode (1); the second conveyor belt (7) bypasses the second guide roller (5) and the third guide roller (8) and is closed on the lower surface of the anode (1); when a first conveyor belt (6) and a second conveyor belt (7) on the surface below an anode (1) enter an intercalation electrolyte (12), two layers of the first conveyor belt (6) and the second conveyor belt (7) are sleeved with a conveyor belt buckle (9), so that the first conveyor belt (6) and the second conveyor belt (7) carry out space limitation and extrusion on the anode (1), and when the first conveyor belt (6) and the second conveyor belt (7) leave an oxidation electrolyte (13), the conveyor belt buckle (9) is taken down, and the pressure borne by the anode (1) is released; the conductive roller (2) is connected with the anode of the power supply (3) through a lead, the intercalation slot cathode group (10) and the oxidation slot cathode group (11) are connected with the cathode of the power supply (3) through leads, and the intercalation slot cathode group (10) and the oxidation slot cathode group (11) are respectively soaked in the intercalation electrolyte (12) and the oxidation electrolyte (13).
2. According to the claimsThe method for preparing graphene oxide by two-step electrochemical continuous electrolysis is characterized in that the graphite raw material is a sheet or a wire prepared from a composite of one or more of natural graphite, artificial graphite, massive graphite, crystalline flake graphite, aphanitic graphite, expanded graphite or graphite powder; the preferred graphite material has a density in the range of 1.0 to 2.0g/cm 3 The flexible graphite paper of (2).
3. The two-step electrochemical continuous electrolysis process for preparing graphene oxide according to claim 1, wherein the conveying device includes but is not limited to one or more combinations of a belt conveyor, a roller conveyor, a chain scraper conveyor, a mesh belt conveyor or a suspension conveyor; the movement rate of the graphite raw material relative to the electrolyte is 0 to 1000m/h, preferably 0.1cm/h to 5m/h.
4. The two-step electrochemical continuous electrolysis method for preparing graphene oxide according to claim 1, wherein the pressure applied by the conveying device to the graphite raw material is constant or variable during the conveying process of the graphite raw material, and the pressure ranges of the graphite raw material during the intercalation reaction and the oxidation reaction are 0-50 MPa and 0-20 MPa respectively.
5. The method for preparing graphene oxide according to the two-step electrochemical continuous electrolysis as claimed in claim 4, wherein the conveying device applies pressure to the graphite raw material by means including but not limited to a mixture of one or more of restriction of expansion space, spring fastening, electric pressurization, hydraulic pressurization or pneumatic pressurization.
6. The method for preparing graphene oxide by two-step electrochemical continuous electrolysis according to claim 1, wherein the electrolytes in the intercalation tank and the oxidation tank are the same or different, and the electrolyte is selected from a mixture of one or more than two non-reactive systems of acid or salt; wherein the acid includes, but is not limited to, sulfuric acid, nitric acid, perchloric acid, phosphoric acid, hydrochloric acid, acetic acid, trifluoroacetic acid, trifluoromethanesulfonic acid, chlorosulfonic acid, or magic acid, and the salt includes, but is not limited to, ammonium sulfate, potassium sulfate, sodium sulfate, magnesium sulfate, potassium perchlorate, or sodium persulfate.
7. The method for preparing graphene oxide through two-step electrochemical continuous electrolysis according to claim 6, wherein the electrolyte mass concentration of the electrolyte in the intercalation tank is in the range of 0.01% to 100%, preferably 60% to 100%; the electrolyte mass range concentration of the electrolyte in the oxidation tank is 0.01-100%, preferably 20-85%.
8. The method for preparing graphene oxide by two-step electrochemical continuous electrolysis according to claim 1, wherein the same or different cathode materials are used in the intercalation tank and the oxidation tank; cathode materials include, but are not limited to, platinum, copper, nickel, gold, or graphite corresponding plates, meshes, wires, or rods; the relative position of the anode and the cathode includes but is not limited to single cathode and single anode facing, two cathodes sandwiching one anode or cathode surrounding the anode, and the surface distance between the anode material and the cathode material is in the range of 0.1 mm-1 m.
9. The two-step electrochemical continuous electrolysis for preparing graphene oxide according to claim 1, wherein the voltage applied between the anode and the cathode is a continuous direct current voltage, a pulsed direct current voltage or an alternating current voltage, and the voltage range is 0.1 to 10kV, preferably 1 to 100V.
10. The method for preparing graphene oxide through two-step electrochemical continuous electrolysis according to claim 1, wherein the anode material after the oxidation reaction is completed is stripped by one or a combination of mechanical shearing, ultrasonic crushing and high-pressure homogenization, and the anode material after the oxidation reaction is completed is cleaned by one or a combination of centrifugal cleaning, filter pressing cleaning and cross-flow cleaning.
CN202211197331.XA 2022-09-29 2022-09-29 Method for continuously preparing graphene oxide through two-step electrochemistry Pending CN115404496A (en)

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