CN108298530A - A kind of form the few-layer graphene alkene and the preparation method and application thereof - Google Patents
A kind of form the few-layer graphene alkene and the preparation method and application thereof Download PDFInfo
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- CN108298530A CN108298530A CN201810043585.3A CN201810043585A CN108298530A CN 108298530 A CN108298530 A CN 108298530A CN 201810043585 A CN201810043585 A CN 201810043585A CN 108298530 A CN108298530 A CN 108298530A
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
- H01M4/583—Carbonaceous material, e.g. graphite-intercalation compounds or CFx
- H01M4/587—Carbonaceous material, e.g. graphite-intercalation compounds or CFx for inserting or intercalating light metals
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
- H01M2004/027—Negative electrodes
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/50—Improvements relating to the production of bulk chemicals
- Y02P20/54—Improvements relating to the production of bulk chemicals using solvents, e.g. supercritical solvents or ionic liquids
Abstract
The present invention provides a kind of form the few-layer graphene alkene and the preparation method and application thereof, which is to utilize CO using natural flake graphite as raw material2Fluid carries out intercalation to the natural flake graphite at supercritical conditions, and intercalation terminates, then be prepared after quick pressure releasing.The industrialized mass production of form the few-layer graphene alkene may be implemented in preparation method provided by the present invention, and its is simple for process, and operating cost is relatively low, and the number of plies of gained form the few-layer graphene alkene is 1 10 layers.The form the few-layer graphene alkene is used as lithium ion battery negative material, relatively low and stable operating voltage can be provided, relative to commercial graphite, under the conditions of identical charge-discharge test, there is broader voltage platform；In addition, in terms of capacity, with superior high rate performance, and all there is higher reversible capacity under different current densities.
Description
Technical field
The present invention relates to a kind of form the few-layer graphene alkene and the preparation method and application thereof, belong to carbon material and its application technology neck
Domain.
Background technology
Lithium ion battery is a kind of new type of energy storage device for having many advantages, such as high-energy density and having extended cycle life.The battery
Mainly it is made of anode, cathode and electrolyte three parts.Wherein, positive electrode include LiFePO4, cobalt acid lithium, LiMn2O4 and
Some tertiary cathode materials, wherein commercial general using LiFePO4；Business negative material is natural graphite.Battery charges
When, the lithium ion that deintercalation goes out in positive electrode is embedded into after electrolyte in negative material, when battery discharge, lithium ion by
Cathode is deviate from and is embedded into positive electrode.For cathode, graphite can provide relatively low and stable operating voltage, and
And it has extended cycle life, coulombic efficiency is also very high；But its theoretical capacity is limited, only 372mA h g-1, this is limited significantly
The raising of lithium ion battery chemical property.
Graphene is a kind of sp with ideal two-dimensional structure2Hydridization new carbon, to constitute graphite flake, carbon nanometer
Pipe and fullerene basic structural unit, and graphene have excellent mechanical property, good electric conductivity and other one
The special electricity of series, optics, calorifics, chemical property；These unique characteristics are it in electronic device and as electrode material
The application of the body phase material of material etc. provides possibility.Relative to graphite, graphene has high-specific surface area and high conductance
The advantages that rate, graphene are formed by the unordered loose aggregate of single layer of carbon atom, this is beneficial to the insertion and abjection of lithium ion, stone
The two-sided of black alkene can store lithium ion, therefore enhance the storage capacity of lithium ion.The theoretical capacity of metal oxidation is higher.
Yoo et al. (Nano Letters 2008；8(8):Performance of the graphene in negative electrode of lithium ion battery 2277-82) is tested,
Electrochemical results show its specific capacity up to 540mA h g-1.Yao et al. (Nanoscale Research Letters
2014；9(1):When 1-6.) the hollow graphite alkene microballoon synthesized is used as negative electrode of lithium ion battery, in 50mA g-1When, reversible appearance
Amount is 903mA h g-1Even if in 500mA h g-1Under, reversible capacity remains to reach 502mA h g-1, and in 50mA g-1
Under electric current after 60 circle of cycle, capacity is 652mA h g-1。
To meet the needs of this field is to lithium ion battery high-energy density, using the graphene with superior electrical conductivity energy
The storage of lithium can be improved as lithium ion battery negative material and enhances the diffusion rate of lithium ion.Therefore it provides a kind of
The excellent graphene of electric conductivity and the technology for having become this field urgent need to resolve as lithium ion battery negative material
Problem.
Invention content
In order to solve above-mentioned disadvantage and deficiency, the purpose of the present invention is to provide a kind of form the few-layer graphene alkene.
The present invention also aims to provide the preparation method of the form the few-layer graphene alkene.
The present invention also aims to provide application of the form the few-layer graphene alkene as lithium ion battery negative material.
The present invention also aims to provide the lithium ion battery electrode slurry containing the form the few-layer graphene alkene.
The present invention also aims to provide the preparation method of the lithium ion battery electrode slurry.
In order to achieve the above objectives, the present invention provides a kind of form the few-layer graphene alkene, which is with natural flake graphite
For raw material, CO is utilized2Fluid carries out intercalation to the natural flake graphite at supercritical conditions, and intercalation terminates, then through quickly letting out
It is prepared after pressure.
According to specific embodiments of the present invention, it is preferable that the number of plies of the form the few-layer graphene alkene is 1-10 layers.
The present invention also provides the preparation methods of the form the few-layer graphene alkene comprising following steps：
(1) it weighs natural flake graphite and adds it in reaction kettle, then inject carbon dioxide into reaction kettle, simultaneously
By in reaction kettle pressure and temperature rise to reaction pressure and reaction temperature respectively so that carbon dioxide reaches supercriticality；
(2) intercalation is carried out after carbon dioxide reaches supercriticality, so that the abundant intercalation of carbon dioxide molecule, is inserted
Layer after reaction, reacting kettle inner pressure is quickly let out to normal pressure to carry out the stripping reaction of graphite layers；
(3) step (1)-(2) are repeated, the form the few-layer graphene alkene is obtained.
According to specific embodiments of the present invention, in the preparation method, it is preferable that the quality of the natural flake graphite
Volume ratio with supercritical carbon dioxide is 1:1-1:5, unit is respectively g and mL.
According to specific embodiments of the present invention, in the preparation method, it is preferable that the time of the intercalation is
30-120min；
According to specific embodiments of the present invention, in the preparation method, it is preferable that the number of the repetition is 5-10
It is secondary.Wherein, it is that realize, repeatedly stripping is anti-by reciprocal pressurising and pressure release that step (1)-(2) are repeated described in step (3)
It answers, one step completed pressurising and pressure leak process are to have carried out a stripping reaction in preparation method provided by the present invention.
According to specific embodiments of the present invention, in the preparation method, it is preferable that the reaction pressure is 10-
20MPa, reaction temperature are 35-50 DEG C.
According to specific embodiments of the present invention, in the preparation method, it is preferable that step waits for intercalation knot in (2)
Shu Hou lets out reacting kettle inner pressure to normal pressure in 1-10s to carry out the stripping reaction of graphite layers.
According to specific embodiments of the present invention, in the preparation method, reaction kettle used is the routine that this field uses
Reaction kettle.
Application the present invention also provides the form the few-layer graphene alkene as lithium ion battery negative material.
According to specific embodiments of the present invention, in the application, it is preferable that the grain size of the form the few-layer graphene alkene is
200-1000 mesh.Wherein, the grain size of form the few-layer graphene alkene is excessive or too small is unfavorable for it as lithium ion battery negative material
Shi Xingneng (such as relatively low and stable operating voltage, broader voltage platform, superior high rate performance and higher reversible appearance
Amount) performance.
The present invention also provides a kind of lithium ion battery electrode slurrys, are made of dispersate and dispersant, with this point
The total weight for dissipating matter is 100% calculating comprising the form the few-layer graphene alkene and surplus (10-50%) conductive black of 50-90%
And binder；
The dispersant is N-methyl pyrrolidones.
Wherein, the application need to only ensure that the sum of the dosage of conductive black and binder is in lithium ion battery electrode slurry
10-50%, and specific requirement is not made to each plant demand of the two, it is reasonable that those skilled in the art can need according to field operation
The concrete content of the two is set, as long as ensureing that the object of the invention may be implemented.
According to specific embodiments of the present invention, in the lithium ion battery electrode slurry, it is preferable that the binder
For vinylidene.
The present invention also provides the preparation methods of the lithium ion battery electrode slurry comprising following steps：
The form the few-layer graphene alkene, conductive black and vinylidene binder are added in N-methyl pyrrolidones, stirring is mixed
It closes uniformly, obtains the lithium ion battery electrode slurry.
The present invention utilizes CO using natural flake graphite as raw material2It is (super that molecule carries out intercalation under conditions of high pressure to graphite
Critical CO2Fluid stripping method utilizes carbon dioxide molecule in the diffusion process at gas-liquid-solid interface, enables carbon dioxide molecule
It is enough to be fast and effeciently inserted into graphite layers), using realizing the layers-separated of graphite flake layer after quick pressure releasing；The present invention is carried
The industrialized mass production of form the few-layer graphene alkene may be implemented in this method of confession, and its is simple for process, and operating cost is relatively low, gained
The number of plies of form the few-layer graphene alkene is 1-10 layers.
The form the few-layer graphene alkene that the present invention is prepared is used as lithium ion battery negative material, can provide relatively low and flat
Steady operating voltage, relative to commercial graphite, under the conditions of identical charge-discharge test, such as under the charging voltage of 0.5V,
With broader voltage platform；In addition, in terms of capacity, with superior high rate performance, and in different electric currents
All there is higher reversible capacity, such as in the specific embodiment of the invention, the lithium ion battery is in 50mA g under density-1Item
Under part, reversible capacity is up to 516mA h g-1, it is far above the capacity of commercial graphite.
Description of the drawings
Fig. 1 is the transmission electron microscope picture for the form the few-layer graphene alkene that the embodiment of the present invention 1 is prepared；
Fig. 2 be the form the few-layer graphene alkene that is prepared of the embodiment of the present invention 1 as lithium ion battery negative material when multiplying power
Performance chart；
Fig. 3 be the form the few-layer graphene alkene that is prepared of the embodiment of the present invention 2 as lithium ion battery negative material when,
150mA g-1Electric current under cycle performance curve graph；
Fig. 4 is the scanning electron microscope (SEM) photograph for the form the few-layer graphene alkene that the embodiment of the present invention 3 is prepared；
Fig. 5 be the form the few-layer graphene alkene that is prepared of the embodiment of the present invention 3 as lithium ion battery negative material when multiplying power
Performance chart；
Fig. 6 is that the form the few-layer graphene alkene that the embodiment of the present invention 4 is prepared and commercial graphite are negative respectively as lithium ion battery
High rate performance curve graph when the material of pole；
Fig. 7 is that the form the few-layer graphene alkene that the embodiment of the present invention 4 is prepared and commercial graphite are negative respectively as lithium ion battery
When the material of pole, in 50mA g-1Electric current under charging and discharging curve figure；
Fig. 8 be the form the few-layer graphene alkene that is prepared of the embodiment of the present invention 5 as lithium ion battery negative material when,
150mA g-1Under charging and discharging curve figure；
Fig. 9 be the form the few-layer graphene alkene that is prepared of the embodiment of the present invention 5 as lithium ion battery negative material when,
500mA g-1Under charging and discharging curve figure.
Specific implementation mode
In order to which technical characteristic, purpose and the advantageous effect to the present invention are more clearly understood, in conjunction in detail below
Embodiment technical scheme of the present invention is carried out it is described further below, but should not be understood as to the present invention can practical range limit
It is fixed.
Embodiment 1
Present embodiments provide a kind of preparation method of form the few-layer graphene alkene comprising following steps：
(1) 20g natural flake graphites are weighed and are added it in reaction kettle, then inject 40mL titanium dioxides into reaction kettle
Carbon, while reacting kettle inner pressure is risen into 15MPa, temperature rises to 35-50 DEG C, so that carbon dioxide reaches supercriticality；
(2) intercalation 30-120min is carried out after carbon dioxide reaches supercriticality, so that carbon dioxide molecule fills
After intercalation, reacting kettle inner pressure is let out to normal pressure in 2s to carry out the stripping reaction of graphite layers for point intercalation；
(3) step (1)-(2) are repeated 9 times, 10 stripping reactions are carried out by reciprocal pressurising and pressure release altogether, are obtained described
Form the few-layer graphene alkene.
Transmission electron microscope analysis is carried out to form the few-layer graphene alkene obtained by the present embodiment, transmission electron microscope picture is as shown in Figure 1, from Fig. 1
In as can be seen that there are the number of plies being 4 layers and 5 layers of graphene in the form the few-layer graphene alkene.
Form the few-layer graphene alkene obtained by the present embodiment is sieved into grain size and is the graphene of 200 mesh, and is used as lithium-ion electric
The assembling of the negative material in pond, the lithium ion battery includes the following steps：
1) according to 8:1:1 mass ratio weighs form the few-layer graphene alkene, conductive black and poly- inclined fluorine prepared by the present embodiment
Ethylene binder makes its uniformly compound, mixing time 10 using N-methyl pyrrolidones as dispersant using magnetic agitation
Hour, obtain slurry；
2) above-mentioned slurry is subjected to even spread with coater on copper foil, then as being dried in 100 DEG C of baking ovens,
Copper foil is cut into the electrode slice of a diameter of 13mm using tablet press machine, the electrode obtained piece is in 110 DEG C of vacuum drying chambers after drying
Dry 12h.Button cell is assembled in the glove box full of argon gas as reference electrode using lithium piece, oxygen and water in glove box
Content be respectively less than 0.1ppm；Simultaneously using the 1mol L dissolved with phosphoric acid vinyl acetate and dimethyl carbonate mixed solution-1LiPF6
As electrolyte, the assembling of lithium ion battery is completed.
Then gained lithium ion battery is tested for the property, test instrument is new Weir charge-discharge test instrument, is surveyed
Examination content includes high rate performance test, charge-discharge characteristic test and cycle performance test, wherein the electricity of constant current charge-discharge test
Pressure range is 0.01-3V (opposite Li/Li+), current density range is 50-1000mA g-1。
High rate performance curve graph when the form the few-layer graphene alkene that the present embodiment is prepared is as lithium ion battery negative material
As shown in Fig. 2, from figure 2 it can be seen that it is in 50mA g-1Electric current under capacity be 467mA h g-1。
Embodiment 2
Present embodiments provide a kind of preparation method of form the few-layer graphene alkene comprising following steps：
(1) 20g natural flake graphites are weighed and are added it in reaction kettle, then inject 40mL titanium dioxides into reaction kettle
Carbon, while reacting kettle inner pressure is risen into 15MPa, temperature rises to 35-50 DEG C, so that carbon dioxide reaches supercriticality；
(2) intercalation 30-120min is carried out after carbon dioxide reaches supercriticality, so that carbon dioxide molecule fills
After intercalation, reacting kettle inner pressure is let out to normal pressure in 2s to carry out the stripping reaction of graphite layers for point intercalation；
(3) step (1)-(2) are repeated 9 times, 10 stripping reactions are carried out by reciprocal pressurising and pressure release altogether, are obtained described
Form the few-layer graphene alkene.
Form the few-layer graphene alkene obtained by the present embodiment is sieved into grain size and is the graphene of 400 mesh, and is used as lithium-ion electric
The negative material in pond, the assembling of the lithium ion battery and test process are the same as embodiment 1, wherein what the present embodiment was prepared
When form the few-layer graphene alkene is as lithium ion battery negative material, in 150mA g-1Electric current under cycle performance curve graph such as Fig. 3
It is shown, from figure 3, it can be seen that it is in 150mA g-1Electric current under cycle 100 circle after capacity be 439mA h g-1, and follow
Capacity is undamped after ring.
Embodiment 3
Present embodiments provide a kind of preparation method of form the few-layer graphene alkene comprising following steps：
(1) 20g natural flake graphites are weighed and are added it in reaction kettle, then inject 40mL titanium dioxides into reaction kettle
Carbon, while reacting kettle inner pressure is risen into 15MPa, temperature rises to 35-50 DEG C, so that carbon dioxide reaches supercriticality；
(2) intercalation 30-120min is carried out after carbon dioxide reaches supercriticality, so that carbon dioxide molecule fills
After intercalation, reacting kettle inner pressure is let out to normal pressure in 2s to carry out the stripping reaction of graphite layers for point intercalation；
(3) step (1)-(2) are repeated 9 times, 10 stripping reactions are carried out by reciprocal pressurising and pressure release altogether, are obtained described
Form the few-layer graphene alkene.
Electron microscope analysis is scanned to form the few-layer graphene alkene obtained by the present embodiment, scanning electron microscope (SEM) photograph is as shown in figure 4, from Fig. 4
In as can be seen that the form the few-layer graphene alkene surfacing, and transparency is higher.
Form the few-layer graphene alkene obtained by the present embodiment is sieved into grain size and is the graphene of 600 mesh, and is used as lithium-ion electric
The negative material in pond, the assembling of the lithium ion battery and test process are the same as embodiment 1, wherein what the present embodiment was prepared
High rate performance curve graph when form the few-layer graphene alkene is as lithium ion battery negative material as shown in figure 5, from figure 5 it can be seen that
It is in 500mA g-1Electric current under capacity be 209mA h g-1。
Embodiment 4
Present embodiments provide a kind of preparation method of form the few-layer graphene alkene comprising following steps：
(1) 20g natural flake graphites are weighed and are added it in reaction kettle, then inject 40mL titanium dioxides into reaction kettle
Carbon, while reacting kettle inner pressure is risen into 15MPa, temperature rises to 35-50 DEG C, so that carbon dioxide reaches supercriticality；
(2) intercalation 30-120min is carried out after carbon dioxide reaches supercriticality, so that carbon dioxide molecule fills
After intercalation, reacting kettle inner pressure is let out to normal pressure in 2s to carry out the stripping reaction of graphite layers for point intercalation；
(3) step (1)-(2) are repeated 9 times, 10 stripping reactions are carried out by reciprocal pressurising and pressure release altogether, are obtained described
Form the few-layer graphene alkene.
Form the few-layer graphene alkene obtained by the present embodiment is sieved into grain size and is the graphene of 800 mesh, and is used as lithium-ion electric
The negative material in pond, while using commercially available commercial graphite (Lishen Battery Co., Ltd., Tianjin) as the negative of lithium ion battery
Pole material；The assembling of the lithium ion battery and test process are the same as embodiment 1, wherein the few layer stone that the present embodiment is prepared
High rate performance curve graph when black alkene and commercial graphite are respectively as lithium ion battery negative material is as shown in fig. 6, the present embodiment
When the form the few-layer graphene alkene and commercial graphite being prepared are respectively as lithium ion battery negative material, in 50mA g-1Electric current
Under charging and discharging curve figure as shown in fig. 7, it can be seen from the figure that form the few-layer graphene alkene is prepared as cathode using the present embodiment
The lithium ion battery that material preparation obtains is in 50mA g-1Electric current under capacity be 516mA h g-1, far above using business stone
Capacity (the 451mA h g of ink-1), and it has broader 0.5V platforms below.
Embodiment 5
Present embodiments provide a kind of preparation method of form the few-layer graphene alkene comprising following steps：
(1) 20g natural flake graphites are weighed and are added it in reaction kettle, then inject 40mL titanium dioxides into reaction kettle
Carbon, while reacting kettle inner pressure is risen into 15MPa, temperature rises to 35-50 DEG C, so that carbon dioxide reaches supercriticality；
(2) intercalation 30-120min is carried out after carbon dioxide reaches supercriticality, so that carbon dioxide molecule fills
After intercalation, reacting kettle inner pressure is let out to normal pressure in 2s to carry out the stripping reaction of graphite layers for point intercalation；
(3) step (1)-(2) are repeated 9 times, 10 stripping reactions are carried out by reciprocal pressurising and pressure release altogether, are obtained described
Form the few-layer graphene alkene.
Form the few-layer graphene alkene obtained by the present embodiment is sieved into grain size and is the graphene of 1000 mesh, and is used as lithium-ion electric
The negative material in pond, the assembling of the lithium ion battery and test process are the same as embodiment 1, wherein what the present embodiment was prepared
When form the few-layer graphene alkene is as lithium ion battery negative material, in 150mA g-1And 500mA g-1Under charging and discharging curve figure point
Not as Figure 8-9, it can be seen from the figure that it is in 150mA g-1With 500mA g-1Electric current under capacity be respectively 410 Hes
252mA h g-1。
In addition, it can also be seen that by form the few-layer graphene provided by the present invention from constant current charge-discharge curve graph (Fig. 7-9)
The charge and discharge process for the lithium ion battery that alkene is prepared as negative material mainly carries out between 0-0.5V, in full battery
System, this will be helpful to obtain a higher operating voltage.
Claims (10)
1. a kind of form the few-layer graphene alkene, which is characterized in that the form the few-layer graphene alkene is to utilize CO using natural flake graphite as raw material2Fluid
Intercalation is carried out to the natural flake graphite at supercritical conditions, intercalation terminates, then be prepared after quick pressure releasing.
2. form the few-layer graphene alkene according to claim 1, which is characterized in that the number of plies of the form the few-layer graphene alkene is 1-10 layers.
3. the preparation method of form the few-layer graphene alkene described in claims 1 or 2 comprising following steps：
(1) it weighs natural flake graphite and adds it in reaction kettle, then inject carbon dioxide into reaction kettle, while will be anti-
Pressure and temperature in kettle is answered to rise to reaction pressure and reaction temperature respectively, so that carbon dioxide reaches supercriticality；
(2) intercalation is carried out after carbon dioxide reaches supercriticality, so that the abundant intercalation of carbon dioxide molecule, intercalation are anti-
After answering, reacting kettle inner pressure is quickly let out to normal pressure to carry out the stripping reaction of graphite layers；
(3) step (1)-(2) are repeated, the form the few-layer graphene alkene is obtained；
Preferably, the time of the intercalation is 30-120min；
It is further preferred that the number of the repetition is 5-10 times.
4. preparation method according to claim 3, which is characterized in that the quality of the natural flake graphite and overcritical two
The volume ratio of carbonoxide is 1:1-1:5, unit is respectively g and mL.
5. preparation method according to claim 3, which is characterized in that the reaction pressure is 10-20MPa, reaction temperature
It is 35-50 DEG C.
6. preparation method according to claim 3, which is characterized in that step waits for intercalation after reaction in (2), will react
Pressure is let out to normal pressure in 1-10s to carry out the stripping reaction of graphite layers in kettle.
7. application of the form the few-layer graphene alkene as lithium ion battery negative material described in claims 1 or 2.
8. application according to claim 7, which is characterized in that the grain size of the form the few-layer graphene alkene is 200-1000 mesh.
9. a kind of lithium ion battery electrode slurry, is made of dispersate and dispersant, which is characterized in that with the dispersate
Total weight is 100% to calculate comprising form the few-layer graphene alkene and surplus conductive black described in claims 1 or 2 of 50-90% and viscous
Tie agent；
The dispersant is N-methyl pyrrolidones；
Preferably, the binder is vinylidene.
10. the preparation method of lithium ion battery electrode slurry described in claim 9 comprising following steps：
N-methyl pyrrolidones is added in form the few-layer graphene alkene, conductive black described in claims 1 or 2 and vinylidene binder
In, it is uniformly mixed, obtains the lithium ion battery electrode slurry.
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN110668433A (en) * | 2019-11-25 | 2020-01-10 | 陕西师范大学 | Method for preparing graphite/graphene composite material by supercritical carbon dioxide fluid and application |
| CN112261858A (en) * | 2020-10-14 | 2021-01-22 | 北京中博视讯科技有限公司 | Graphene composite material and preparation method and application thereof |
| CN114188532A (en) * | 2021-11-09 | 2022-03-15 | 中国石油大学(北京) | Graphene negative electrode material and preparation method and application thereof |
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