CN113991085A - Carbon-silicon material and preparation method of carbon-silicon-carbon material - Google Patents

Carbon-silicon material and preparation method of carbon-silicon-carbon material Download PDF

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CN113991085A
CN113991085A CN202111260902.5A CN202111260902A CN113991085A CN 113991085 A CN113991085 A CN 113991085A CN 202111260902 A CN202111260902 A CN 202111260902A CN 113991085 A CN113991085 A CN 113991085A
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silicon
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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
    • H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
    • 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
    • H01M4/362—Composites
    • H01M4/366—Composites as layered products
    • 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
    • H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
    • H01M4/386—Silicon or alloys based on silicon
    • 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
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H01M4/624—Electric conductive fillers
    • H01M4/625—Carbon or graphite
    • 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

Abstract

The invention discloses a carbon-silicon material and a preparation method of the carbon-silicon-carbon material, which comprises porous carbon and silicon-containing gas; placing porous carbon in a container, heating the porous carbon, and heating the porous carbon to a temperature at which silicon-containing gas is decomposed into silicon ions, hydrogen ions or/and chloride ions; when the porous carbon in the container is processed to the required temperature, the gas containing silicon is sent into the container, and the silicon ions decomposed by the silicon gas are combined or mixed on the surface or/and in the holes of the porous carbon through nucleation and growth again to form the carbon-silicon composite or/and mixed material with the porous carbon. The material prepared by the invention can restrict the expansion and cracking of silicon when being applied to the lithium ion battery cathode material, and simultaneously provides a space gap for the expansion of the silicon, so that the silicon material can be effectively applied to the lithium ion battery cathode material.

Description

Carbon-silicon material and preparation method of carbon-silicon-carbon material
Technical Field
The invention relates to a carbon-silicon material and a preparation method of the carbon-silicon-carbon material.
Background
With the development progress of globalization, the human society enters the era of digitalization, 5G, new energy automobile, energy storage and 3D printing, the application of superfine powder synthetic materials is more and more, and particularly, in order to realize international manufacturing strong country in the automobile industry of China, the goal of realizing the goal of developing new energy automobiles into curve overtaking is adopted in China; however, lithium ion power battery materials adopted by the existing lithium ion new energy automobile, particularly high-end high-grade carbon-silicon composite or/and mixed materials, are imported by developed countries in the United states, America and Europe to provide goods sources in China.
In order to solve the urgent need of the required nanoscale carbon-silicon cathode material, the research personnel adopt a physical gas phase method to prepare a finer nanoscale composite material, which is a future development direction and an inevitable trend, in the face of the existing chemical method for preparing an ultrafine powder material, because the ultrafine powder material has serious environmental pollutants, great danger and extremely high manufacturing cost, and the capacity cannot be industrially produced in large quantities; the resource content of silicon in the earth crust is extremely rich, the lithium storage capacity of the silicon is 4200mah/g theoretically, the current lithium battery cathode materials commonly used in China at present all adopt graphite carbon materials, the theoretical lithium storage capacity is 372mah/g, the silicon is 10 times of the lithium storage capacity of the current graphite carbon cathode materials, and the silicon is a preferred application material in the future all around when being used as a high-end cathode material of a lithium ion battery; however, in the lithium ion charging and discharging processes, the volume expansion of silicon is about 300% during lithium insertion, which causes cracking and crushing of the electrode, and finally causes separation of the electrode material from the current collector, which seriously affects the electrochemical stability of the electrode, and easily reduces the battery capacity to a large extent, so that it is very important to solve the problem.
Disclosure of Invention
The present invention is directed to solve the problems of the background art, and provides a carbon-silicon material and a method for preparing the carbon-silicon-carbon material.
In order to solve the technical problems, the technical scheme of the invention is as follows: a carbon-silicon material and a preparation method of the carbon-silicon-carbon material are characterized in that: comprises porous carbon and silicon-containing gas; placing porous carbon in a container, heating the porous carbon, and heating the porous carbon to a temperature at which silicon-containing gas is decomposed into silicon ions, hydrogen ions or/and chloride ions; when the porous carbon in the container is processed to the required temperature, the gas containing silicon is sent into the container, and the silicon ions decomposed by the silicon gas are combined or mixed on the surface or/and in the holes of the porous carbon through nucleation and growth again to form the carbon-silicon composite or/and mixed material with the porous carbon.
In the above carbon-silicon material and the preparation method of the carbon-silicon-carbon material, the carbon-silicon composite or/and mixed material and the graphite cathode material are uniformly mixed in a weight ratio of 5% -85%: 95-15% of the carbon-silicon composite or/and mixed material is independently applied to the cathode material of the lithium ion battery with extra high capacity.
In the above carbon-silicon material and the preparation method of the carbon-silicon-carbon material, the surface or/and the holes of the carbon-silicon composite or/and mixed material formed by the porous carbon are/is further coated with one or/and multiple layers of conductor materials to form the carbon-silicon-carbon composite or/and mixed material, which is applied to the negative electrode material of the lithium ion battery.
In the above carbon-silicon material and the preparation method of the carbon-silicon-carbon material, the silicon-containing gas is dichlorosilane or monosilane.
In the above-mentioned carbon-silicon material and the preparation method of the carbon-silicon-carbon material, the porous carbon is heated to a temperature that can cause the silicon-containing gas to generate heat to decompose silicon ions, hydrogen ions or/and chloride ions, and the heating temperature is greater than 100-2000 ℃.
In the above carbon-silicon material and the preparation method of the carbon-silicon-carbon material, the silicon ions are re-nucleated, grown, combined or/and mixed on the surface or/and in the pores of the porous carbon to form a composite or/and mixed material of the silicon-containing element material, wherein the weight percentage of the composite or/and mixed material of the silicon-containing element material to the porous carbon material is 0.1-5: 1.
In the above-mentioned carbon-silicon material and preparation method of carbon-silicon-carbon material, the carbon-silicon composite or/and mixed material formed by porous carbon is added into the solution to be dispersed, or more than one material of aldehyde resin, glucose, sucrose, starch, poly (acrylonitrile), polymethacrylate, polyvinyl chloride resin and asphalt is added synchronously or later to be uniformly emulsified or ultrasonically or vibrationally dispersed and mixed, and then the mixture is filtered, dried or spray-dried or dried, and then placed in a container, and then the container is heated to the temperature of 620 ℃ and 1300 ℃ in a heating furnace, and finally the carbon-silicon-carbon composite or/and mixed material is obtained after 1-24 hours of carbonization treatment.
In the above-mentioned carbon-silicon material and the preparation method of the carbon-silicon-carbon material, the carbon-silicon composite or/and mixed material formed by the porous carbon is processed and crushed into the granular powder and added into the space capable of heating and decomposing the hydrocarbon gas, the hydrocarbon gas in the heating and decomposing space is decomposed and simultaneously generates hydrogen ions and carbon ions, and the temperature of the thermal decomposition space is above 600 ℃; and (3) the carbon ions are re-nucleated, adsorbed and coated on the surface and in the holes of the carbon-silicon composite or/and mixed particle powder material to form a carbon coating layer, so that the carbon-silicon-carbon composite or/and mixed material is obtained.
In the above-mentioned carbon-silicon material and preparation method of carbon-silicon-carbon material, the hydrocarbon gas is introduced into the carbon-silicon composite or/and mixed material formed by porous carbon, and heated to a temperature above 630 ℃ to decompose the hydrocarbon gas into carbon ions and hydrogen ions, so that the carbon ions are recombined and grown on the surface of the carbon-silicon composite or/and mixed material, thereby obtaining the carbon-silicon-carbon composite or/and mixed material.
In the above carbon-silicon material and the preparation method of the carbon-silicon-carbon material, the carbon-silicon-carbon composite or/and mixed material and the graphite negative electrode material are uniformly mixed in a weight ratio of 5% -85%: 95-15% of the carbon-silicon-carbon composite or/and mixed material is independently applied to the cathode material of the lithium ion battery with the ultrahigh capacity. .
In the above carbon-silicon material and the preparation method of the carbon-silicon-carbon material, the hydrocarbon gas is: methane, ethane, propane, ethylene, acetylene, propylene, propyne gas.
In the above carbon-silicon material and the preparation method of the carbon-silicon-carbon material, the average pore size of the pores of the porous carbon is 2nm-1000nm, and the volume ratio of the pores to the total volume of the pores is 20% -90%.
In the above carbon-silicon material and the preparation method of the carbon-silicon-carbon material, the composite or/and mixed material of the silicon-containing material is elemental silicon or/and silicon oxide or/and silicon carbide or/and silicon nitride, for example: silicon monoxide, silicon carbide, silicon nitride, pure silicon, and the like.
In the above carbon-silicon material and the preparation method of the carbon-silicon-carbon material, the porous carbon may be graphitized or/and soft carbon or/and hard carbon.
In the above carbon-silicon material and the preparation method of the carbon-silicon-carbon material, the porous carbon may also be carbon nanotubes or/and carbon fibers.
In the above carbon-silicon material and the preparation method of the carbon-silicon-carbon material, the porous carbon heating is resistance heating or arc heating.
In the above carbon-silicon material and the preparation method of the carbon-silicon-carbon material, the porous carbon is heated by induction heating.
In the above carbon-silicon material and the preparation method of the carbon-silicon-carbon material, the porous carbon heating is dielectric heating.
In the above carbon-silicon material and the preparation method of the carbon-silicon-carbon material, the silicon-containing gas is trichlorosilane or silicon tetrachloride.
The invention has the following beneficial effects:
according to the invention, porous carbon and silicon-containing gas are heated, the porous carbon and silicon ions decomposed by heating are mixed to form a carbon-silicon composite or/and mixed material, and the carbon-silicon composite or/and mixed material is coated with one or/and multiple layers of carbon layers to form a carbon-silicon-carbon composite or/and mixed material which is applied to a lithium ion battery cathode material; the material prepared by the invention can restrict the expansion and cracking of silicon when being applied to the lithium ion battery cathode material, and simultaneously provides a space gap for the expansion of the silicon, so that the silicon material can be effectively applied to the lithium ion battery cathode material.
Detailed Description
The invention is further illustrated below.
A carbon-silicon material and a preparation method of the carbon-silicon-carbon material are characterized in that: comprises porous carbon and silicon-containing gas; placing porous carbon in a container, heating the porous carbon, and heating the porous carbon to a temperature at which silicon-containing gas is decomposed into silicon ions, hydrogen ions or/and chloride ions; when the porous carbon in the container is processed to the required temperature, the gas containing silicon is sent into the container, and the silicon ions decomposed by the silicon gas are combined or mixed on the surface or/and in the holes of the porous carbon through nucleation and growth again to form the carbon-silicon composite or/and mixed material with the porous carbon.
Further, the carbon-silicon composite or/and mixed material and the graphite cathode material are uniformly mixed in a weight ratio of 5% -85%: 95-15% of the carbon-silicon composite or/and mixed material is independently applied to the cathode material of the lithium ion battery with extra high capacity.
Further, the surface or/and the holes of the carbon-silicon composite or/and mixed material formed by the porous carbon are/is further coated with one or/and multiple layers of conductor materials, such as: carbon, metal material and nitride material, thereby forming carbon-silicon-carbon composite or/and mixed material which is applied to the lithium ion battery cathode material.
Further, the silicon-containing gas is dichlorosilane or monosilane.
Further, the porous carbon is heated to a temperature which can cause the silicon-containing gas to generate thermal decomposition to obtain silicon ions, hydrogen ions or/and chloride ions, and the heating temperature is more than 100-2000 ℃.
Further, the silicon ions are combined or/and mixed in the surface or/and the holes of the porous carbon to form a composite or/and mixed material of the silicon-containing element material, wherein the weight percentage of the composite or/and mixed material of the silicon-containing element material to the porous carbon material is 0.1-5: 1.
Further, adding the carbon-silicon composite or/and mixed material formed by porous carbon into the solution for dispersion, or synchronously or later adding more than one of aldehyde resin, glucose, sucrose, starch, poly (acrylonitrile), polymethacrylate, polyvinyl chloride resin and asphalt for uniform emulsification or ultrasonic or oscillation dispersion and mixing, filtering, drying or spray drying or drying, placing the mixture into a container, putting the container into a heating furnace, heating to the temperature of 620-1300 ℃, and carrying out carbonization treatment for 1-24 hours to obtain the carbon-silicon-carbon composite or/and mixed material.
Further, the carbon-silicon composite or/and mixed material formed by the porous carbon is processed and crushed into particle powder, the particle powder is added into a space capable of heating and decomposing hydrocarbon gas, the hydrocarbon gas in the heating and decomposing space is decomposed and simultaneously generates hydrogen ions and carbon ions, and the temperature of the thermal decomposition space is more than 600 ℃; and (3) the carbon ions are re-nucleated, adsorbed and coated on the surface and in the holes of the carbon-silicon composite or/and mixed particle powder material to form a carbon coating layer, so that the carbon-silicon-carbon composite or/and mixed material is obtained.
Further, hydrocarbon gas is introduced into the carbon-silicon composite or/and mixed material formed by the porous carbon, and is heated to a temperature of above 630 ℃, so that the hydrocarbon gas is decomposed into carbon ions and hydrogen ions, and the carbon ions are recombined and grow on the surface of the carbon-silicon composite or/and mixed material, and further the carbon-silicon-carbon composite or/and mixed material is obtained.
Further, the carbon-silicon-carbon composite or/and mixed material and the graphite cathode material are uniformly mixed in a weight ratio of 5% -85%: 95-15% of the carbon-silicon-carbon composite or/and mixed material is independently applied to the cathode material of the lithium ion battery with the ultrahigh capacity. .
Further, the hydrocarbon gas is: methane, ethane, propane, ethylene, acetylene, propylene, propyne gas.
Further, the average pore size of the pores of the porous carbon is 2nm-1000nm, and the average pore size accounts for 20% -90% of the total pore volume.
Further, the composite or/and mixed material of the material containing the silicon element is simple substance silicon or/and silicon oxide or/and silicon carbide or/and silicon nitride, such as: silicon monoxide, silicon carbide, silicon nitride, pure silicon, and the like.
Further, the porous carbon may be graphitized or/and soft carbon or/and hard carbon.
Further, the porous carbon can also adopt carbon nano tubes or/and carbon fibers.
Further, the porous carbon heating is resistance heating or arc heating.
Further, the porous carbon heating is induction heating.
Further, the porous carbon heating is dielectric heating.
Further, the silicon-containing gas is trichlorosilane or silicon tetrachloride.
The invention is further described below in terms of specific examples for better understanding, but some of the contents are simplified for easier reading and implementation.
Example 1:
weighing 6 kilograms of porous carbon, putting the porous carbon into a container with the average pore diameter of 266nm and the pore volume ratio of 58 percent, heating the porous carbon to 660 ℃ through a resistor, sending silane gas into the container at the flow rate of 1 cubic meter per hour, and generating silicon ions and hydrogen ions through heating and decomposition; silicon ions are grown on the surface and in holes of the porous carbon in situ for 1 hour and 36 minutes, and the carbon-silicon composite material is taken out after cooling, so that about 12 kilograms of the carbon-silicon composite material is obtained, and the carbon-silicon material is crushed to 0.5-38 microns to form a granular cathode material with the average grain diameter of 22 microns to be made into a button cell;
the charge-discharge test is carried out at the current of 0.1C, the charge-discharge test shows that the first coulombic efficiency of the detection result reaches 85.6 percent, the first discharge specific capacity is 2156mAh/g, the first charge specific capacity is 1845.6mAh/g, the capacity after 500-week circulation is kept to 85 percent, the 1000-time circulation capacity is kept to 75 percent, the nearly 2000-time circulation capacity is kept to nearly 67 percent, the circulation performance is excellent and is close to the top level of the same industry in China, 13 percent floats under the circulation performance of the existing full graphite cathode material compared with the existing full graphite cathode material, and the first capacity is about 6.25 times of the existing graphite cathode capacity of about 330mAh/g-365 mAh/g.
Example 2:
weighing 6 kg of porous carbon nanofiber, placing the porous carbon nanofiber into a container with the average pore diameter of 106nm and the pore volume ratio of 55%, heating the porous carbon to 660 ℃ through resistance, sending monosilane gas into the container at the flow rate of 1 cubic meter per hour, and heating and decomposing the monosilane gas to generate silicon ions and hydrogen ions; the silicon ions are grown on the surface and in the holes of the porous carbon in situ for 1 hour and 36 minutes, and the carbon-silicon composite material is taken out after cooling, so that about 12 kilograms of the carbon-silicon composite material is obtained, and the carbon-silicon material is crushed to 0.5-50 microns to form particles of about 1: 1;
taking 1 kg, adding the crushed carbon-silicon composite material particles into an organic ethanol solution for uniform emulsification and dispersion, adding 1 kg of glucose, drying the filtrate, putting the dried carbon-silicon composite material containing glucose powder into a high-temperature furnace, carbonizing the grape at 830 ℃ for 5 hours, cooling to normal temperature, taking out the product to obtain the carbon-silicon-carbon high-capacity cathode material of which the weight is about 1.28 kg, and crushing to obtain the cathode material of 3-25um to prepare the button cell;
through charge and discharge tests at 0.1C current, the detection result is obtained, the first coulombic efficiency reaches 92%, the first discharge specific capacity is 1660mAh/g, the first charge specific capacity is 1527mAh/g, the capacity after 500-week circulation is 91%, the 1000-time circulation capacity is 83%, the nearly 2000-time circulation capacity is nearly 68%, the circulation performance is excellent and is close to the top level of the international industry, and the 12% first capacity of the existing full-graphite cathode material floating under the circulation performance is about 4.5-5 times of the existing graphite cathode capacity of 330mAh/g-365 mAh/g.
Example 3:
weighing 6 kg of porous carbon nanotubes, filling the porous carbon nanotubes into a container, heating the porous carbon nanotubes to 75% by volume through a medium, heating the porous carbon nanotubes to 1056 ℃, sending trichlorosilane gas into the container at a flow rate of 1 cubic per hour, heating and decomposing the trichlorosilane gas to generate silicon ions, hydrogen ions and chloride ions, wherein the silicon ions are grown on the surface and in the holes of the porous carbon in situ for 1 hour, cooling and taking out the carbon-silicon composite material to obtain the carbon-silicon composite material with the weight of about 11.38 kg, and the carbon-silicon ratio is about 1: 0.86, crushing the carbon-silicon material into particles of 0.5-50 um;
taking 1 kg, adding crushed carbon-silicon composite material particles into an organic ethanol solution for uniform emulsification and dispersion, adding 1 kg of glucose, drying the filtrate, putting the dried carbon-silicon composite material containing glucose powder into a high-temperature furnace, carbonizing a grape at 830 ℃ for 5 hours, cooling to normal temperature, taking out the product to obtain a carbon-silicon-carbon high-capacity cathode material of which the weight is about 1.28 kg, and crushing to obtain a 3-25um cathode material to prepare a button cell;
the charge-discharge test is carried out under the current of 0.1C, the first coulombic efficiency of the obtained detection result reaches 89%, the first discharge specific capacity is 1366mAh/g, the first charge specific capacity is 1216mAh/g, the capacity after 500-week circulation is kept to 89% and 1000 times, the circulation capacity is kept to 79%, the circulation capacity is kept to be excellent at nearly 61% for nearly 2000 times, the capacity floats to 19% under the good circulation performance compared with the existing all-graphite cathode material, and the first capacity is about 3 times of the existing graphite cathode capacity of 330mAh/g-365 mAh/g.
Example 4:
weighing 6 kg of porous carbon, putting the porous carbon into a container, heating the porous carbon to 660 ℃ by induction heating, sending monosilane gas into the container at a flow rate of 1 cubic meter per hour, heating and decomposing to generate silicon ions and hydrogen ions, taking the silicon ions in situ on the surface and in holes of the porous carbon for 1 hour for 36 minutes, cooling and taking out the carbon-silicon composite material to obtain about 12 kg of the carbon-silicon composite material, and forming about 1: 1;
the carbon-silicon composite material is heated to 968 ℃, methane gas is sent into the carbon-silicon composite material at the flow rate of 0.1 cubic meter per hour, the carbon-silicon composite material is cooled to normal temperature after 106 minutes, the carbon-silicon-carbon high-capacity negative electrode material is taken out to be about 1.28 kilograms, and the carbon-silicon-carbon high-capacity negative electrode material is crushed to obtain 3-25um negative electrode material to be made into a button cell;
through charge and discharge tests at 0.1C current, the detection result is obtained, the first coulombic efficiency reaches 94%, the first discharge specific capacity is 1660mAh/g, the first charge specific capacity is 1560mAh/g, the capacity after 500-week circulation is kept to 92.5%, the circulation capacity is kept to 86% after 1000 times, the circulation capacity is kept to nearly 75% after nearly 2000 times, the circulation performance is excellent and is close to the top level of the international same industry, and the 5% first discharge specific capacity floated under the circulation performance of the existing full-graphite negative electrode material is nearly 4.65-5.16 times of the existing graphite negative electrode capacity which is about 330mAh/g-365 mAh/g.
Example 5:
the carbon-silicon-carbon negative electrode material in the example 1 and the commercially available high-end graphitized negative electrode material are mixed by 35%: 65 percent of the total components are mixed and prepared into a button cell for testing, the first coulombic efficiency reaches 93 percent, the first discharge specific capacity is about 818mAh/g, and the first charge specific capacity is 761.5 mAh/g. The specific discharge capacity after 500-week cyclic charge and discharge is 92.5%, the specific discharge capacity after 1000-week cyclic charge and discharge is 86%, and the specific discharge capacity after 2000-week cyclic charge and discharge is 78.5%.
The carbon-silicon material and the preparation method of the carbon-silicon-carbon material provided by the embodiment of the invention are described in detail, and the principle and the implementation mode of the invention are explained by applying specific examples, and the description of the embodiment is only used for helping to understand the technical scheme disclosed by the invention; meanwhile, for a person skilled in the art, according to the idea of the present invention, there may be variations in the specific embodiments and the application scope, and in summary, the content of the present specification should not be construed as a limitation of the present invention.

Claims (19)

1. A carbon-silicon material and a preparation method of the carbon-silicon-carbon material are characterized in that: comprises porous carbon and silicon-containing gas;
placing porous carbon in a container, heating the porous carbon, and heating the porous carbon to a temperature at which silicon-containing gas is decomposed into silicon ions, hydrogen ions or/and chloride ions;
when the porous carbon in the container is processed to the required temperature, the gas containing silicon is sent into the container, and the silicon ions decomposed by the silicon gas are combined or mixed on the surface or/and in the holes of the porous carbon through nucleation and growth again to form the carbon-silicon composite or/and mixed material with the porous carbon.
2. The preparation method of carbon-silicon material and carbon-silicon-carbon material according to claim 1, characterized in that: the carbon-silicon composite or/and mixed material and the graphite cathode material are uniformly mixed in a weight ratio of 5-85%: 95-15% of the carbon-silicon composite or/and mixed material is independently applied to the cathode material of the lithium ion battery with extra high capacity.
3. The preparation method of carbon-silicon material and carbon-silicon-carbon material according to claim 1, characterized in that: and the surface or/and the holes of the carbon-silicon composite or/and mixed material formed by the porous carbon are/is further coated with one or/and multiple layers of conductor materials to form the carbon-silicon-carbon composite or/and mixed material which is applied to the negative electrode material of the lithium ion battery.
4. The preparation method of carbon-silicon material and carbon-silicon-carbon material according to claim 1, characterized in that: the silicon-containing gas is dichlorosilane or monosilane.
5. The preparation method of carbon-silicon material and carbon-silicon-carbon material according to claim 1, characterized in that: the porous carbon is heated to a temperature which can cause the silicon-containing gas to generate thermal decomposition to obtain silicon ions, hydrogen ions or/and chloride ions, and the heating temperature is more than 100-2000 ℃.
6. The preparation method of carbon-silicon material and carbon-silicon-carbon material according to claim 1, characterized in that: the silicon ions are combined or/and mixed in the surface or/and the holes of the porous carbon to form a composite or/and mixed material of the silicon-containing element material, wherein the weight percentage of the composite or/and mixed material of the silicon-containing element material to the porous carbon material is 0.1-5: 1.
7. The preparation method of carbon-silicon material and carbon-silicon-carbon material according to claim 3, characterized in that: adding the carbon-silicon composite or/and mixed material formed by porous carbon into the solution for dispersion, or synchronously or later adding more than one of aldehyde resin, glucose, sucrose, starch, poly (acrylonitrile), polymethacrylate, polyvinyl chloride resin and asphalt for uniform emulsification or ultrasonic or oscillation dispersion and mixing, filtering, drying or spray drying or drying, placing the mixture into a container, entering a heating furnace, heating to the temperature of 620-1300 ℃, and carrying out carbonization treatment for 1-24 hours to obtain the carbon-silicon-carbon composite or/and mixed material.
8. The preparation method of carbon-silicon material and carbon-silicon-carbon material according to claim 3, characterized in that: processing and crushing carbon-silicon composite or/and mixed materials formed by the porous carbon into particle powder, adding the particle powder into a space capable of heating and decomposing hydrocarbon gas, heating and decomposing the hydrocarbon gas in the space, and simultaneously generating hydrogen ions and carbon ions, wherein the temperature of the thermal decomposition space is more than 600 ℃; and (3) the carbon ions are re-nucleated, adsorbed and coated on the surface and in the holes of the carbon-silicon composite or/and mixed particle powder material to form a carbon coating layer, so that the carbon-silicon-carbon composite or/and mixed material is obtained.
9. The preparation method of carbon-silicon material and carbon-silicon-carbon material according to claim 3, characterized in that: and introducing hydrocarbon gas into the carbon-silicon composite or/and mixed material formed by the porous carbon, heating to the temperature of above 630 ℃, decomposing the hydrocarbon gas into carbon ions and hydrogen ions, recombining the carbon ions and growing the carbon ions on the surface of the carbon-silicon composite or/and mixed material, and further obtaining the carbon-silicon-carbon composite or/and mixed material.
10. The carbon-silicon material and the preparation method of the carbon-silicon-carbon material according to claim 7, 8 or 9, wherein the preparation method comprises the following steps: the carbon-silicon-carbon composite or/and mixed material and the graphite cathode material are uniformly mixed according to the weight ratio of 5% -85%: 95-15% of the carbon-silicon-carbon composite or/and mixed material is independently applied to the cathode material of the lithium ion battery with the ultrahigh capacity.
11. The preparation method of carbon-silicon material and carbon-silicon-carbon material according to claim 8, wherein the preparation method comprises the following steps: the hydrocarbon gas is: methane, ethane, propane, ethylene, acetylene, propylene, propyne gas.
12. The preparation method of carbon-silicon material and carbon-silicon-carbon material according to claim 1, characterized in that: the average pore diameter of the pores of the porous carbon is 2nm-1000nm, and the average pore diameter accounts for 20% -90% of the total pore volume.
13. The carbon-silicon material and the preparation method of the carbon-silicon-carbon material according to claim 1 are characterized in that: the composite or/and mixed material of the material containing the silicon element is simple substance silicon or/and silicon oxide or/and silicon carbide or/and silicon nitride, such as: silicon monoxide, silicon carbide, silicon nitride, pure silicon, and the like.
14. The carbon-silicon material and the preparation method of the carbon-silicon-carbon material according to claim 1 are characterized in that: the porous carbon may be graphitized or/and soft carbon or/and hard carbon.
15. The carbon-silicon material and the preparation method of the carbon-silicon-carbon material according to claim 1 are characterized in that: the porous carbon can also adopt carbon nano tubes or/and carbon fibers.
16. The carbon-silicon material and the preparation method of the carbon-silicon-carbon material according to claim 1 are characterized in that: the porous carbon heating is resistance heating or electric arc heating.
17. The carbon-silicon material and the preparation method of the carbon-silicon-carbon material according to claim 1 are characterized in that: the porous carbon heating adopts induction heating.
18. The carbon-silicon material and the preparation method of the carbon-silicon-carbon material according to claim 1 are characterized in that: the porous carbon heating is medium heating.
19. The carbon-silicon material and the preparation method of the carbon-silicon-carbon material according to claim 1 are characterized in that: the silicon-containing gas is trichlorosilane or silicon tetrachloride.
CN202111260902.5A 2021-10-28 2021-10-28 Carbon-silicon material and preparation method of carbon-silicon-carbon material Pending CN113991085A (en)

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