CN109761228A - The method and apparatus of two-dimensional material are efficiently removed under a kind of low reynolds number - Google Patents

The method and apparatus of two-dimensional material are efficiently removed under a kind of low reynolds number Download PDF

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CN109761228A
CN109761228A CN201910246708.8A CN201910246708A CN109761228A CN 109761228 A CN109761228 A CN 109761228A CN 201910246708 A CN201910246708 A CN 201910246708A CN 109761228 A CN109761228 A CN 109761228A
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dimensional material
body phase
reynolds number
microchannel
suspension
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CN109761228B (en
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袁学锋
袁松洋
兰扎罗
张绍林
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Guangzhou University
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Abstract

The present invention relates to a kind of methods that two-dimensional material is efficiently removed under low reynolds number, and macromolecule and surfactant are added into solvent, and arrival adds two-dimensional sheet granular materials after being completely dissolved and obtains the suspension of body phase two-dimensional material, macromolecule and surfactant;By suspension by the micro flow chip equipped with microchannel, suspension flow at high speed in microchannel generates turbulent flow, generates very high shearing force between the vortex in turbulent flow, to make the removing of body phase two-dimensional material at the two-dimensional material of single layer or few layer.The method overcome efficiency low yields in conventional two-dimensional material stripping process, it is difficult to the problems such as being mass produced, while can realize the efficient removing of body phase two-dimensional material under relatively low pressure, be a kind of very promising two-dimensional material stripping means.The device for efficiently removing two-dimensional material under a kind of low reynolds number is further related to, material processing preparation field is belonged to.

Description

The method and apparatus of two-dimensional material are efficiently removed under a kind of low reynolds number
Technical field
The present invention relates to materials to process preparation field, efficiently removes two-dimensional material under specifically a kind of low reynolds number Method and apparatus.
Background technique
Two-dimensional material including graphene has wide with its excellent and diversified material property in many fields Application prospect, including sensor, field effect transistor, laser, electrolysis water, battery and capacitor area etc..A large amount of section Worker has done many research in the research of two-dimensional material and application aspect, wherein being effectively peeled off for two-dimensional material is to grind The first step with engineer application two-dimensional material is studied carefully, because only that two-dimensional material is many excellent in the case where single layer or few layer Performance is likely to display.Currently, the method that common two-dimensional material is removed includes mechanical stripping, and ultrasound centrifugation, polishing Deng, but these stripping means are all there is some problems, such as low efficiency, low yield, and power consumption is big, it is difficult to large-scale production etc., Find a kind of energy-efficient, the two-dimensional material stripping means of high yield is always one of the content of many scientific workers' researchs. Cambridge University's graphene research center Andrea C.Ferrari team is once by graphene aqueous solution in microchannel, in high pressure Under conditions of high flow rate, graphene is removed using the powerful shearing force generated between being vortexed in turbulent flow inertia area, has obtained high concentration, The graphene single layer solution of 100% yield.But this method condition is harsh, needs under high pressure (2000 atmospheric pressure) It carries out, experiment condition is required in practical operation high.
Summary of the invention
For the technical problems in the prior art, the object of the present invention is to provide efficiently shell under a kind of low reynolds number Method from two-dimensional material, this method can be under relatively low pressure and Reynolds number, and efficiently removing obtains including graphene Two-dimensional material inside.The method overcome efficiency low yields in conventional two-dimensional material stripping process, it is difficult to large-scale production etc. Problem, while can realize the efficient removing of two-dimensional material under relatively low pressure, before there are good industrial applications Scape.
It is a further object of the present invention to provide two-dimentional material is efficiently removed under a kind of low reynolds number for realizing the above method The device of material.
In order to achieve the above object, the present invention adopts the following technical scheme:
Macromolecule and surfactant are added into solvent for a kind of method that two-dimensional material is efficiently removed under low reynolds number, Arrival adds two-dimensional sheet granular materials after being completely dissolved and obtains the suspension of body phase two-dimensional material, macromolecule and surfactant Liquid;By suspension by the micro flow chip equipped with microchannel, suspension flow at high speed in microchannel generates turbulent flow, turbulent flow In vortex between generate very high shearing force, to make the removing of body phase two-dimensional material at the two-dimensional material of single layer or few layer.
Preferably, macromolecule refers to the flexible polymer of the dissolution of the water-soluble or organic solvent with high molecular weight, as body The turbulence induced agent of phase two-dimensional material suspension makes body phase two-dimensional material suspension induce generation rapid under lower Reynolds number Stream obtains the two-dimensional material of single layer or few layer to realize efficiently removing.
Preferably, it is outstanding to be that single layer or few layer two-dimensional sheet granular materials after avoiding removing reassembles for surfactant Supernatant liquid stabilizer.
Preferably, the body phase two-dimensional material after microchannel is removed flows back again is delivered to microchannel and is shelled again From recirculation gas stripper is until remove the two-dimensional material at single layer or few layer.
Preferably, the multiple parameters of device and the property of body phase two-dimensional material suspension are adjusted, Kolmogorov long is adjusted The size of degree, to adjust the size range for being suitable for turbulent flow removing two-dimensional material indirectly.
Preferably, by changing the planform of microchannel, and then stripping conditions are adjusted.
The device that two-dimensional material is efficiently removed under a kind of low reynolds number, including micro flow chip, the condensing unit set gradually And material placing device, micro flow chip are equipped with microchannel, further include for body phase two-dimensional material suspension to be sent into micro flow chip Pressure pump;Body phase two-dimensional material suspension is flowed in microchannel high speed generates turbulent flow, between the small vortex in turbulent flow Shearing force removes body phase two-dimensional material.
Preferably, microchannel is the beeline channel that cluster is parallel to each other.
Preferably, microchannel is the interior channel for having several cylindrical structures perpendicular to fluid flow direction of flat lamelliform.
It preferably, further include for being automatically fed into the material feeding system for being mixed with high molecular body phase two-dimensional material suspension.
It preferably, further include reflux unit, one end of reflux unit connects material placing device, and one end connects material feeding system, returns Stream device is used to the body phase two-dimensional material in material placing device being delivered to material feeding system, removed again through microchannel to single layer or The two-dimensional material of few layer.
The principle of the present invention is: in microchannel, using the property of Polymer Solution, in relatively low pressure and Reynolds Under several, efficiently removing obtains the two-dimensional material including graphene.High score has been dissolved in the suspension of body phase two-dimensional material Son, turbulence induced agent of the macromolecule as body phase two-dimensional material suspension, Polymer Solution is in flow process, due to macromolecule What is generated is unstable, therefore is more prone to produce turbulent flow, thus in relatively low flow velocity, under lower Reynolds number, realization pair The removing of two-dimensional material.Simultaneously because the drag reduction effect of Polymer Solution may be implemented compared to Newtonian fluid relatively low Pressure under, generate high flow rate, help to realize so at lower pressures efficiently removing body phase two-dimensional material.
Generally speaking, the present invention has the advantage that
1. due to joined macromolecule in the suspension of body phase two-dimensional material, macromolecule suspends as body phase two-dimensional material The turbulence induced agent of liquid is brought at low pressures and the advantages of compared with body phase two-dimensional material is effectively peeled off under low reynolds number.Phase Compared with the stripping means of existing condition harshness, experiment condition of the invention is easier to realize.
2. the present invention realizes energy-efficient production using micro-fluidic method.All almost due to all body phase two-dimensional materials Under identical stripping conditions, therefore the uniformity of obtained product is more preferable, and yield is higher.
Detailed description of the invention
Fig. 1 is the schematic device of present invention removing body phase two-dimensional material.
Fig. 2 is the structural schematic diagram of micro flow chip.
Label and corresponding parts title in figure are as follows: 1- material feeding system, 2- body phase two-dimensional material, 3- pressure pump, 4- Vortex, 5- micro flow chip, 6- microchannel, 7- condensing unit, 8- material placing device, the two-dimensional material of 9- single layer or few layer, 10- are returned Flow device.
Specific embodiment
Below with reference to examples and drawings, the present invention will be further described in detail, but embodiments of the present invention are not It is limited to this.
It is body phase two-dimensional material before removing in the present invention, is the two-dimensional material of single layer or few layer after removing.
The device of two-dimensional material is efficiently removed under a kind of low reynolds number, as shown in Figure 1, including material feeding system, pressure pump, micro- Flowing chip, condensing unit, reflux unit and material placing device, condensing unit is condenser.Material feeding system is mixed with for being automatically fed into High molecular body phase two-dimensional material suspension, the body phase two-dimensional material suspension that material feeding system is sent by pressure pump pass through miniflow core Piece and condensing unit are delivered to material placing device, and the body phase two-dimensional material suspension in material placing device is sent into pan feeding by reflux unit System realizes multiple recirculation gas stripper, finally obtains the two-dimensional material of single layer or few layer.Body phase in body phase two-dimensional material suspension Two-dimensional material is that (unstripped material or the insufficient material of removing are known as body phase two-dimensional material, remove for the two-dimensional material of multilayer Single layer or few layer (i.e. 5 layers or less) afterwards is known as doing two-dimensional material), micro flow chip is equipped with microchannel, due to pressure pump It is pumped into, body phase two-dimensional material suspension flow at high speed in microchannel generates turbulent flow, can generate very between the vortex in turbulent flow High shearing force, to make the removing of body phase two-dimensional material at the two-dimensional material of single layer or few layer.In the stripping process of microchannel In, all body phase two-dimensional materials are all exposed under high shearing force simultaneously, and all body phase two-dimensional materials can be simultaneously Removing, therefore obtained product uniformity is more preferable, can achieve 100% yield.And in traditional stripping means, only leaning on Place (this is small part in entire solution/suspension) meeting of nearly rotor (mechanical stripping) or amplitude transformer (ultrasound removing) Generating enough power makes the removing of body phase two-dimensional material at single layer or few layer, therefore yield is very low, is usually no more than 1%, and compare Compared with energy consumption.Two-dimensional material after microchannel is removed is after condensing unit condenses, into material placing device;Stripping in material placing device It is sent into material feeding system by reflux unit from insufficient body phase two-dimensional material suspension, realizes recirculation gas stripper, it is ensured that removing is filled Point.
Due to high molecular addition, body phase two-dimensional material suspension can be made to induce generation rapid under lower Reynolds number Stream, shape the having an impact less to turbulent flow of fluid channel, the shape of fluid channel can be set as different patterns.So of the invention The microchannel of device uses simple shape, the beeline channel being parallel to each other in the present embodiment using cluster.
The device of the invention can be effectively peeled off the realization of body phase two-dimensional material by adjusting multiple parameters, comprising: miniflow The radius in channel, surface roughness, the shape of cross section, Fluid pressure;Single or plurality of passages are parallel, improve efficiency;Micro- Cylinder or square column etc. are added in circulation road, cylinder or square column are used to form around column stream, also induce turbulent flow around column stream, and then design The condition more conducively removed.
A kind of method that two-dimensional material is efficiently removed under low reynolds number, is realized using above-mentioned apparatus, is included the following steps:
(1) a certain amount of macromolecule and surfactant are added into solvent, arrival adds a certain amount of after being completely dissolved Two-dimensional sheet granular materials obtain the suspension of body phase two-dimensional material, macromolecule and surfactant;What the present invention was added Macromolecule refers to the flexible polymer of the dissolution of the water-soluble or organic solvent with high molecular weight, and main function is as two-dimentional material The turbulence induced agent of pulp suspension, can induce suspension compared under low reynolds number just generate turbulent flow, to remove two-dimensional material. It in the present embodiment, takes water as a solvent, macromolecule is by taking PAAM molecular weight 18,000,000 as an example, concentration 0.01wt%;Two-dimensional material with For graphene (removing to obtain with graphite), graphite concentration 10mg/ml;By taking CTAB as an example, concentration is surfactant 0.22mg/ml.The concentration of macromolecule, surfactant and body phase two-dimensional material is adjustable to obtain better peeling effect, It is not restricted to described in the present embodiment.
(2) multiple parameters of device and the property of body phase two-dimensional material suspension are adjusted, Kolmogorov length is adjusted Size, to adjust the size range for being suitable for turbulent flow removing two-dimensional material indirectly.Wherein adjust body phase two-dimensional material suspension Property include adjust body phase two-dimensional material suspension viscosity, density, flow velocity, surface tension, the row of macromolecule in a solvent Except bulk effect, high molecular molecular weight, molecular weight distribution and concentration, the concentration etc. of the body phase two-dimensional material of addition.Wherein fill The multiple parameters set include: the radius of microchannel, surface roughness, the shape of cross section, Fluid pressure;Single is a plurality of logical Road is parallel, improves efficiency;Cylinder or square column etc. are added in microchannel.
(3) suspension that step (1) obtains is sent to microchannel, Polymer Solution from material feeding system using pressure pump With turbulent flow drag reduction effect, compared to Newtonian fluid, may be implemented at a pressure that is relatively low, to generate high velocity stream, body phase two It ties up material suspension flow at high speed in microchannel and generates turbulent flow, very high shearing force can be generated between the vortex in turbulent flow, To remove body phase two-dimensional material.
(4) two-dimensional material after step (3) removing enters material placing device after condenser condenses.
(5) it for insufficient body phase two-dimensional material is removed, can be re-fed by reflux unit in microchannel again Secondary removing, multiple recirculation gas stripper obtain the two-dimensional material of single layer or few layer, it is ensured that removing is abundant.
The present invention uses micro-fluidic method, realizes efficiently removing.It is micro-fluidic to refer to control fluid (pressure, flow velocity, miniflow The shape etc. in channel) it is flowed in subtle runner, the then behavior of Study of Fluid.In microchannel, the pressure of fluid, flow velocity Substantially it can keep constant, the flow regime (being primarily referred to as turbulent flow) of fluid remains unchanged, since fluid entire in fluid channel is all Turbulent flow, so thering is vortex to generate (turbulent flow can inherently generate vortex) in entire fluid and being produced using between vortex and vortex Raw shearing force removes two-dimensional material, is thus in identical stripping conditions (because entire fluid is all in fluid channel Turbulent flow has vortex to generate).
As long as flow velocity is sufficiently high, so that it may vortex is generated, and since the viscoelastic properties of macromolecule in solvent itself is easy to lure Hair flows unstable, therefore is easier induction and generates turbulent flow, i.e., compared with Newtonian fluid (such as pure water), relatively low Pressure, (i.e. Reynolds number is also low) can generate turbulent flow under flow conditions.
Microflow control technique is easier to control pressure flow velocity of fluid in runner etc., and (because smaller, design is also relatively more square Just), and higher pressure and flow velocity can be reached.
Other than the mode that above-described embodiment refers to, microchannel can also be in the runner of flat lamelliform and be added vertically Cylindrical structure (i.e. in Fig. 2 shown in black origin), cylinder or square column be used to form around column stream, also induce turbulent flow around column stream, this The microfluidic channel design of sample is conducive to increase surface area, improves charge stripping efficiency.These mapping modes are in protection model of the invention In enclosing.
The above embodiment is a preferred embodiment of the present invention, but embodiments of the present invention are not by above-described embodiment Limitation, other any changes, modifications, substitutions, combinations, simplifications made without departing from the spirit and principles of the present invention, It should be equivalent substitute mode, be included within the scope of the present invention.

Claims (10)

1. efficiently removing the method for two-dimensional material under a kind of low reynolds number, it is characterised in that: macromolecule and table are added into solvent Face activating agent, arrival add two-dimensional sheet granular materials and obtain body phase two-dimensional material, macromolecule and surface work after being completely dissolved The suspension of property agent;Suspension is passed through into the micro flow chip equipped with microchannel, suspension high velocity stream movable property in microchannel Turbulent flow is given birth to, generates very high shearing force between the vortex in turbulent flow, to make the removing of body phase two-dimensional material into single layer or lack layer Two-dimensional material.
2. efficiently removing the method for two-dimensional material under low reynolds number described in accordance with the claim 1, it is characterised in that: macromolecule is Refer to the flexible polymer that there is the water-soluble or organic solvent of high molecular weight to dissolve, the turbulent flow as body phase two-dimensional material suspension lures Agent is led, body phase two-dimensional material suspension is induced under lower Reynolds number and generates turbulent flow, to realize efficiently removing, obtains list The two-dimensional material of layer or few layer.
3. efficiently removing the method for two-dimensional material under low reynolds number described in accordance with the claim 1, it is characterised in that: logical through miniflow Body phase two-dimensional material after road removing flow back again to be delivered to microchannel and is removed again, and recirculation gas stripper is until remove into list The two-dimensional material of layer or few layer.
4. efficiently removing the method for two-dimensional material under low reynolds number described in accordance with the claim 1, it is characterised in that: adjustment device Multiple parameters and body phase two-dimensional material suspension property, the size of Kolmogorov length is adjusted, to adjust indirectly suitable Size range for turbulent flow removing two-dimensional material.
5. efficiently removing the method for two-dimensional material under low reynolds number described in accordance with the claim 1, it is characterised in that: pass through change The planform of microchannel, and then adjust stripping conditions.
6. efficiently removing the device of two-dimensional material under a kind of low reynolds number, it is characterised in that: including set gradually micro flow chip, Condensing unit and material placing device, micro flow chip are equipped with microchannel, further include for body phase two-dimensional material suspension to be sent into The pressure pump of micro flow chip;Body phase two-dimensional material suspension is flowed in microchannel high speed generates turbulent flow, the small whirlpool in turbulent flow Shearing force between stream removes body phase two-dimensional material.
7. the device of two-dimensional material is efficiently removed under low reynolds number according to claim 6, it is characterised in that: microchannel The beeline channel being parallel to each other for cluster.
8. the device of two-dimensional material is efficiently removed under low reynolds number according to claim 6, it is characterised in that: microchannel To there is the channel of several cylindrical structures perpendicular to fluid flow direction in flat lamelliform.
9. the device of two-dimensional material is efficiently removed under low reynolds number according to claim 6, it is characterised in that: further include using In being automatically fed into the material feeding system for being mixed with high molecular body phase two-dimensional material suspension.
10. the device of two-dimensional material is efficiently removed under low reynolds number according to claim 9, it is characterised in that: further include Reflux unit, one end of reflux unit connect material placing device, and one end connects material feeding system, and reflux unit is used for will be in material placing device Body phase two-dimensional material be delivered to material feeding system, remove the two-dimensional material to single layer or few layer again through microchannel.
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