CN104882590A - Preparation method of carbon/ graphite/ silicon composited anode material - Google Patents
Preparation method of carbon/ graphite/ silicon composited anode material Download PDFInfo
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- CN104882590A CN104882590A CN201510336207.0A CN201510336207A CN104882590A CN 104882590 A CN104882590 A CN 104882590A CN 201510336207 A CN201510336207 A CN 201510336207A CN 104882590 A CN104882590 A CN 104882590A
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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
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/139—Processes of manufacture
- H01M4/1393—Processes of manufacture of electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
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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
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/362—Composites
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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
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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
Abstract
The invention relates to a preparation method of a carbon/ graphite/ silicon composited anode material. The method is that raw materials are prepared according to the following particle size and percentage by weight: 1.5 to 2.5% of carbon black, 5 to 8% of not greater than 1mm natural graphite, 3 to 10% of not greater than 100nm nanometer silicon, 25 to 30% of not greater than 0.075mm calcined petrol coke powder, 15 to 20% of 1-4mm calcined petrol coke, 10 to 15% of 4 to 10mm electrically calcined anthracite, 5 to 15% of 10 to 16mm calcined pitch coke, and 18 to 20% of coal pitch; short carbon fibers are 1 to 3% according to the total quantity of the raw materials above. The method comprises the steps of mixing the materials; mixing and kneading; calcinating; graphitizing; crushing; spherifying to obtain the carbon/ graphite/ silicon composited material. According to the method, the advantages of the carbon material, graphite material and silicon powder used as the anode materials are combined; therefore, the prepared composited material has the characteristics of being high in the first capacity, high in the first charge-discharge efficiency, and resistant to an electrolyte solvent and isotropy.
Description
Technical field
The present invention relates to a kind of preparation method of charcoal/graphite/silicon composite cathode material, belong to technical field of lithium ion.
Background technology
Since the beginning of the nineties in last century, Sony energy technology company took the lead in successfully developing the lithium ion battery using Carbon anode, lithium ion battery captures rapidly civil secondary Battery Market with the speed of average annual 15%, has become the first-selected power supply of current portable electronic equipment.The develop rapidly of lithium ion battery mainly has benefited from the contribution of electrode material, the particularly progress of negative material.Lithium ion battery negative material requires to possess following characteristics: 1. alap electrode potential; 2. ion has higher diffusivity in negative pole solid-state structure; 3. the deintercalation invertibity of height; 4. good conductivity and thermodynamic stability; 5. security performance is good; 6. good with electrolyte solvent compatibility; 7. aboundresources, cheap, environmentally safe.Negative material is one of large raw material (positive pole, negative pole, electrolyte, barrier film) of lithium ion battery four, what current commercial Li-ion battery negative material adopted is graphite-like material with carbon element, having lower lithium embedding/deintercalation current potential, suitable reversible capacity and aboundresources, the advantage such as cheap, is more satisfactory lithium ion battery negative material.
Inexpensive with it, the nontoxic and superior chemical property of material with carbon element is widely used in lithium ion battery, and state of interface and the fine structure of itself have a great impact electrode performance.At present, commercial carbon negative electrode material of lithium ion cell can be divided into graphite, hard carbon and soft carbon three class, and wherein graphite type material is still the main flow of lithium ion battery negative material.Graphite-like material with carbon element, having lower lithium embedding/deintercalation current potential, suitable reversible capacity and aboundresources, the advantage such as cheap, is more satisfactory lithium ion battery negative material.But its theoretical specific capacity only has 372mAh/g, thus limit the further raising of lithium ion battery specific energy, the demand of growing high-energy Portable power source can not be met.Meanwhile, when graphite is as negative material, in first charge-discharge process, form one deck solid electrolyte film (SEI) on its surface.Solid electrolyte film is the formation that react to each other such as electrolyte, negative material and lithium ion, irreversibly consumes lithium ion, is to form the main factor of of irreversible capacity; It two is in the process of Lithium-ion embeding, electrolyte easily and its be embedded in the process of moving out altogether, electrolyte is reduced, the gaseous product generated causes graphite flake layer to peel off, especially containing in the electrolyte of PC, graphite flake layer comes off new for formation interface, causes further SEI to be formed, irreversible capacity increases, and cyclical stability declines simultaneously.As lithium ion battery negative material, material with carbon element still exists that charge/discharge capacity is low, first cycle irreversible loss is large, solvent molecule intercalation and the shortcoming such as preparation cost is high altogether, and these are also the key issues solved needed in current Study on Li-ion batteries.
Carbon fiber is a kind of novel material with carbon element, divides mainly contain PAN base carbon fibre (on market, more than 90% is this kind of carbon fiber), viscose-based carbon fiber, asphalt base carbon fiber etc. three kinds by raw material.In general, the resistivity of asphalt base carbon fiber is less than PAN base carbon fibre, and PAN base carbon fibre resistivity is less than viscose-based carbon fiber.Electronics rate all can reduce along with the rising of heat treatment temperature.
Chinese patent CN 102623704A, by adding carbon fiber, utilize its high conductivity and strong adsorptivity to prepare lithium carbonate-carbon fiber composite negative pole material to solve the problem of material high rate charge-discharge performance and raising conductivity, meet the requirement of modern society to lithium ion battery applications.Chinese patent CN 102290582A, by adding nanometer overlength carbon fiber VGCF, improving battery conductive, reducing internal resistance.
A kind of tin/graphene/carbon fiber composite lithium cell cathode material preparation method that Chinese patent CN 104037393A announces, the network configuration that Graphene and carbon fiber mixing are formed, for lithium ion turnover electrode provides a large amount of transfer passages smoothly, make it fully contact with negative material, improve the utilization ratio of negative material.Improve the transport velocity of lithium during active position and the discharge and recharge of negative material storage lithium.The high conduction performance of Graphene and carbon fiber can realize carrier mobility fast, effectively can reduce the internal resistance of battery itself while improving power output.
Silicon is a kind of negative material being hopeful to replace material with carbon element most, this is because silicon has the peak capacity up to 4200mAh/g; And there is the stable discharge platform being similar to graphite.But with other high power capacity Metal Phase seemingly, the non-constant of cycle performance of silicon, can not carry out normal charge and discharge cycles.When silicon uses as negative material, in charge and discharge cycles process, the reversible generation of Li2Si alloy and decomposition are along with huge change in volume, the mechanical disintegration of alloy (producing crack and efflorescence) can be caused, cause the avalanche of material structure and peeling off of electrode material and make electrode material lose electrical contact, thus cause the cycle performance of electrode sharply to decline, finally cause electrode failure, therefore in lithium-ions battery, be difficult to practical application.Research shows, the silicon of small particle diameter or its alloy all improve a lot on capacity or on cycle performance, when the particle of alloy material reaches nanoscale, volumetric expansion in charge and discharge process can alleviate greatly, performance also can increase, but nano material has larger surface energy, easily reunites, efficiency for charge-discharge can be made on the contrary to reduce and accelerate the decay of capacity, thus counteract the advantage of nano particle; The silicon fiml adopting various deposition process to prepare can extend the cycle life of material to a certain extent, but can not eliminate the irreversible capacity first that it is higher, thus constrain the practical of this material.Another research tendency improving silicium cathode performance is exactly prepare composite material or the alloy of silicon and other material, and wherein, the silicon/carbon composite prepared in conjunction with the stability of material with carbon element and the height ratio capacity characteristic of silicon shows huge application prospect.
Summary of the invention
The technical problem to be solved in the present invention is to provide a kind of preparation method of charcoal/graphite/silicon composite cathode material, and the negative material that the method prepares has high-pressure solid performance, high connductivity and high rate capability, and long circulating performance.
For solving above technical problem, the technical solution used in the present invention is:
A kind of preparation method of charcoal/graphite/silicon composite cathode material, raw material adopts following granularity and percentage by weight batching: carbon black 1.5-2.5%, ≤ 1mm native graphite 5-8%, ≤ 100nm nano-silicon 3-10% ,≤0.075mm calcined petroleum coke powder 25-30%, 1 ~ 4mm calcined petroleum coke 15-20%, 4 ~ l0mm electric calcined anthracite 10-15%, 10-16mm electric calcined anthracite 5 ~ 10%, 10-16mm calcines pitch coke 5 ~ 15%, coal tar pitch 18-20%; Chopped carbon fiber is 1 ~ 3% of above raw material total amount.
Calcined petroleum coke powder and calcined petroleum coke form through about 1300 DEG C of calcinings.
Electric calcined anthracite forms through more than about 1100-2000 DEG C temperature calcination.
Calcining pitch coke forms through about 1300 DEG C of calcinings.
Carbon black is conductive black, acetylene carbon black, semi-reinforcing hydrocarbon black and relevant carbon black, and performance index are close with the common carbon brush carbon black feed stock of production.
Native graphite can be crystalline flake graphite also can be the amorphous graphite of low ash, and performance index are with to produce common electromechanics carbon and graphite products natural graphite starting material close.
Coal tar pitch can be medium temperature coal pitch can also be modified coal asphalt.
A preparation method for charcoal/graphite/silicon composite cathode material, its preparation process comprises:
(1) batching, kneading, first carry out combined ingredient by carbon black, native graphite, nano-silicon, calcined petroleum coke powder, calcined petroleum coke, electric calcined anthracite and chopped carbon fiber, heat mediate after being dry mixed with coal-tar bond, forms composite plastic gonosome;
(2) roasting, directly loads baking furnace by composite plastic gonosome, through 900-1100 DEG C of roasting, makes carbon material;
(3) graphitization, loads graphitizing furnace by carbon material, through 2200-3000 DEG C of high-temperature process, and obtained charcoal/graphite/silicon composite;
(4) pulverize, nodularization, charcoal/graphite/silicon composite is carried out pulverize, nodularization, obtains spherical or oval charcoal/graphite/silicium cathode powder that particle diameter D50 is 8 ~ 25 μm.
As preferred technical scheme, described kneading, first carbon black, native graphite, nano-silicon, calcined petroleum coke powder, calcined petroleum coke, electric calcined anthracite and calcining pitch coke are added in kneading machine, add chopped carbon fiber again after interval 5-6 minute to be dry mixed, the time of being dry mixed is 35-40 minute, and being dry mixed temperature is 120-150 DEG C; When being dry mixed temperature and reaching time and the temperature of setting, the coal tar pitch adding 175 DEG C-185 DEG C carries out wet mixing, the wet mixing time is at 30-50 minute, kneading temperature is 160-165 DEG C, thickener after kneading is carried out cool material, when thickener temperature is down to 125-145 DEG C, adds in mould and form composite plastic gonosome.
As preferred technical scheme, described carbon fiber is PAN base chopped carbon fiber or asphaltic base chopped carbon fiber.
Described chopped carbon fiber length can be 10-200mm, and average diameter is 5 μm-30 μm.Organic solvent was adopted in advance, as alcohol, acetone etc. carry out dispersion treatment before carbon fiber being added kneading machine.
Lithium ion battery is a kind of rechargeable battery, it mainly rely on lithium ion between a positive electrode and a negative electrode movement carry out work.In charge and discharge process, Li
+come and go between two electrodes and embed and deintercalation: during rechargable battery, Li
+from positive pole deintercalation, embed negative pole through electrolyte, negative pole is in rich lithium state; Then contrary during electric discharge.And graphite cathode material is owing to having good layer structure, be applicable to the embedding-deviate from and form Intercalation reaction formula compound L iC of lithium
x, and there is good charge and discharge platform, be therefore subject to extensive use.And graphite is as lithium ion battery negative material, rushing in electric process first, graphite and electrolyte interface can generate SEI film by interfacial reaction, cause the loss of irreversible capacity, therefore, the theoretical capacity of graphite cathode material is 372mAh/g, but in actual use, its capacity plays and is generally 330 ~ 360 mAh/g, lower than theoretical capacity.And the specific area that SEI film produces irreversible capacity loss and the graphite cathode material caused has direct relation, the specific area of graphite is large, and the scope of electrolyte and graphite contact is large, and the SEI of generation is too much, and the irreversible capacity loss caused is also larger.Meanwhile, because graphite is especially in the electrolyte containing PC, easy and electrolyte occurs embedding altogether, and causes graphite flake layer to peel off, and forms new end face, causes further SEI to be formed, cause cycle performance constantly to reduce.Therefore, the graphite coat modification generally adopted at present, excessive for the specific area of graphite exactly and carry out coated one deck modified layer to reduce the specific area of material, thus improve the discharging efficiency first of graphite, promote its capacity and play and stable circulation performance.
By the Combined Processing to multiple Carbon Materials and material with carbon element presoma and nano-silicon, obtained charcoal/graphite/silicon composite, not only avoid low-crystallinity Carbon Materials capacity low, irreversible capacity loss is large first, next avoids graphite material and embedding altogether and degradation shortcoming under causing cycle performance occurs in organic solvent, composite material effectively can alleviate the bulk effect of silicon in charging process simultaneously, by in conjunction with Carbon Materials and graphite type material and silica flour as respective advantage during negative material, it is high that composite material prepared by the present invention has capacity first, first charge-discharge efficiency is high, electrolyte resistance solvent, the features such as isotropism.Production technology of the present invention is simple simultaneously, excellent product performance, can large-scale production.
Embodiment
Embodiment 1
Batching is :≤1mm micro crystal graphite 5% ,≤100nm nano-silicon 5% ,≤0.075mm calcined petroleum coke 26%, 1 ~ 4mm calcined petroleum coke 15%, 4 ~ l0mm electric calcined anthracite 10%, 10-16mm electric calcined anthracite 5%, 10-16mm calcines pitch coke 14%, acetylene carbon black 2%, coal tar pitch 18%.The T300PAN chopped carbon fiber (diameter 12 μm, length 10mm) of additional above raw material weight 1%, preparation process is as follows:
(1) batching, kneading, first add in kneading machine by carbon black, native graphite, nano-silicon, calcined petroleum coke powder, calcined petroleum coke, electric calcined anthracite and calcining pitch coke, the time of being dry mixed is 35 minutes, and being dry mixed temperature is 120 DEG C; When being dry mixed temperature and reaching time and the temperature of setting, the coal tar pitch adding 175 DEG C carries out wet mixing, and the wet mixing time, kneading temperature was 160 DEG C at 30 minutes, forms composite plastic gonosome;
(2) roasting, loads baking furnace by green, through 1100 DEG C of roastings, makes carbon material;
(3) graphitization, loads graphitizing furnace by carbon material, through 2500 DEG C of high-temperature process, and obtained charcoal/graphite/silicon composite;
(4) pulverize, nodularization, charcoal/graphite/silicon composite is carried out pulverize, nodularization, obtains spherical or oval charcoal/graphite/silicium cathode powder that particle diameter D50 is 12.53 μm.
Embodiment 2
Batching is :≤1mm micro crystal graphite 5% ,≤100nm nano-silicon 10% ,≤0.075mm calcined petroleum coke 25%, 1 ~ 4mm calcined petroleum coke 13%, 4 ~ l0mm electric calcined anthracite 8%, 10-16mm electric calcined anthracite 5%, 10-16mm calcines pitch coke 14%, acetylene carbon black 2%, coal tar pitch 18%.Additional 1% T300PAN chopped carbon fiber (diameter 12 μm, length 10mm), preparation process is as follows:
(1) batching, kneading, first carbon black, native graphite, nano-silicon, calcined petroleum coke powder, calcined petroleum coke, electric calcined anthracite and calcining pitch coke are added in kneading machine, add chopped carbon fiber again after interval 5-6 minute to be dry mixed, the time of being dry mixed is 35 minutes, and being dry mixed temperature is 120 DEG C; When being dry mixed temperature and reaching time and the temperature of setting, the coal tar pitch adding 175 DEG C carries out wet mixing, and the wet mixing time, kneading temperature was 160 DEG C at 30 minutes, forms composite plastic gonosome;
(2) roasting, loads baking furnace by green, through 1100 DEG C of roastings, makes carbon material;
(3) graphitization, loads graphitizing furnace by carbon material, through 2500 DEG C of high-temperature process, and obtained carbon graphite composite material;
(4) pulverize, nodularization, charcoal/graphite/silicon composite is carried out pulverize, nodularization, obtains spherical or oval charcoal/graphite/silicium cathode powder that particle diameter D50 is 11.63 μm.
Embodiment 3
Adopt embodiment 2 to prepare burden constant, additional 2% T300PAN chopped carbon fiber (diameter 12 μm, length 10mm), technique is as embodiment 1.
Embodiment 4
Adopt embodiment 2 to prepare burden constant, additional 3%T300PAN chopped carbon fiber (diameter 12 μm, length 10mm), technique is as embodiment 2.
Embodiment 5
Adopt embodiment 2 to prepare burden constant, respectively additional 3% asphaltic base chopped carbon fiber (diameter 20 μm, length 10mm), technique is as embodiment 2.
Embodiment 6
Batching is: 0.1mm micro crystal graphite 8% ,≤100nm nano-silicon 7%, 0.01mm calcined petroleum coke 25%, 1mm calcined petroleum coke 15%, 4mm electric calcined anthracite 10%, 10mm electric calcined anthracite 5.5%, 10mm calcining pitch coke 10%, acetylene carbon black 1.5%, coal tar pitch 18%.Additional 2%T300PAN chopped carbon fiber (diameter 5 μm, length 200mm).Chopped carbon fiber being added kneading machine adopted organic solvent-acetone to carry out dispersion treatment in the past in advance, preparation process is as follows:
(1) batching, kneading, first carbon black, native graphite, nano-silicon, calcined petroleum coke powder, calcined petroleum coke, electric calcined anthracite and calcining pitch coke are added in kneading machine, interval adds chopped carbon fiber again and is dry mixed after 6 minutes, the time of being dry mixed is 40 minutes, and being dry mixed temperature is 150 DEG C; When being dry mixed temperature and reaching time and the temperature of setting, the coal tar pitch adding 185 DEG C carries out wet mixing, and the wet mixing time was at 50 minutes, kneading temperature is 165 DEG C, thickener after kneading is carried out cool material, when thickener temperature is down to 125 DEG C, adds in mould and form composite plastic gonosome;
(2) roasting, loads baking furnace by green, through 1000 DEG C of roastings, makes carbon material;
(3) graphitization, loads graphitizing furnace by carbon material, through 2500 DEG C of high-temperature process, and obtained carbon graphite composite material;
(4) pulverize, nodularization, charcoal/graphite/silicon composite is carried out pulverize, nodularization, obtains spherical or oval charcoal/graphite/silicium cathode powder that particle diameter D50 is 13.94 μm.
Electrochemical property test
For the performance of negative material prepared by inspection the inventive method, test by half-cell method of testing, negative material by above embodiment: acetylene black: PVDF(Kynoar)=93:3:4(weight ratio), add appropriate NMP(N-methyl pyrrolidone) furnishing pulpous state, coat on Copper Foil, within 8 hours, make negative plate through vacuum 110 DEG C of dryings; Be to electrode with metal lithium sheet, electrolyte is 1mol/L LiPF6/EC+DEC+DMC=1:1:1, and microporous polypropylene membrane is barrier film, is assembled into battery.Charging/discharging voltage is 0 ~ 2.0V, and charge-discharge velocity is 0.2C, and carry out testing to battery performance, test result is in table 1.
Table 1
In order to detect the cycle performance of negative material of the present invention in battery, adopting and being prepared into the detection that 4244130 type Soft Roll resultant battery carry out discharge and recharge.
Negative material by embodiment: SP:SBR(solid content 50%): CMC=94:2.5:1.5:2(weight ratio), add appropriate amount of deionized water and mix furnishing pulpous state, be applied on Copper Foil, at 90 DEG C, vacuumize drying; By LiFePO4 powder: SP:KS-6:PVDF=92:3.5:2:2.5(weight ratio), do after solvent evenly sizes mixing with NMP, be applied on aluminium foil, at 100 DEG C, vacuumize drying; By dried positive and negative electrode pole piece through roll-in, cut-parts, winding, fluid injection, sealing, formation process, make LiFePO4 power type 4244130 type Soft Roll resultant battery (nominal capacity is 2.5Ah), barrier film is Celgard2400, electrolyte is 1M LiPF6 ∕ DMC:EC:DEC, use battery check device to carry out the detection of cycle performance, test result is in table 2.
Table 2
More than show and describe general principle of the present invention, principal character and advantage of the present invention.The technical staff of the industry should understand; the present invention is not restricted to the described embodiments; what describe in above-described embodiment and specification just illustrates principle of the present invention; without departing from the spirit and scope of the present invention; the present invention also has various changes and modifications, and these changes and improvements all fall in the claimed scope of the invention.Claimed scope of the present invention is defined by appending claims and equivalent thereof.
Claims (5)
1. the preparation method of charcoal/graphite/silicon composite cathode material, it is characterized in that: carbon black 1.5-2.5%, ≤ 1mm native graphite 5-8%, ≤ 100nm nano-silicon 3-10% ,≤0.075mm calcined petroleum coke powder 25-30%, 1 ~ 4mm calcined petroleum coke 15-20%, 4 ~ l0mm electric calcined anthracite 10-15%, 10-16mm electric calcined anthracite 5 ~ 10%, 10-16mm calcines pitch coke 5 ~ 15%, coal tar pitch 18-20%; Chopped carbon fiber is 1 ~ 3% of above raw material total amount, and step comprises:
(1) batching, kneading, first carry out combined ingredient by carbon black, native graphite, nano-silicon, calcined petroleum coke powder, calcined petroleum coke, electric calcined anthracite and chopped carbon fiber, heat mediate after being dry mixed with coal-tar bond, forms composite plastic gonosome;
(2) roasting, directly loads baking furnace by composite plastic gonosome, through 900-1100 DEG C of roasting, makes carbon material;
(3) graphitization, loads graphitizing furnace by carbon material, through 2200-3000 DEG C of high-temperature process, and obtained charcoal/graphite/silicon composite;
(4) pulverize, nodularization, charcoal/graphite/silicon composite is carried out pulverize, nodularization, obtains spherical or oval charcoal/graphite/silicium cathode powder that particle diameter D50 is 8 ~ 25 μm.
2. method according to claim 1, it is characterized in that: the kneading described in step (1), first carbon black, native graphite, nano-silicon, calcined petroleum coke powder, calcined petroleum coke, electric calcined anthracite and calcining pitch coke are added in kneading machine, add chopped carbon fiber again after interval 5-6 minute to be dry mixed, the time of being dry mixed is 35-40 minute, and being dry mixed temperature is 120-150 DEG C; When being dry mixed temperature and reaching time and the temperature of setting, the coal tar pitch adding 175 DEG C-185 DEG C carries out wet mixing, the wet mixing time is at 30-50 minute, kneading temperature is 160-165 DEG C, thickener after kneading is carried out cool material, when thickener temperature is down to 125-145 DEG C, adds in mould and form composite plastic gonosome.
3. method according to claim 1, is characterized in that: described carbon fiber is PAN base chopped carbon fiber or asphaltic base chopped carbon fiber.
4. the method according to claim 1 or 6, is characterized in that: described chopped carbon fiber length can be 10-200mm, and average diameter is 5 μm-30 μm.
5. method according to claim 1 and 2, is characterized in that: before chopped carbon fiber being added kneading machine, adopt organic solvent to carry out dispersion treatment in advance.
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