CN108963187A - Silicon-carbon cathode, preparation method, lithium ion battery and electric vehicle - Google Patents
Silicon-carbon cathode, preparation method, lithium ion battery and electric vehicle Download PDFInfo
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Abstract
The invention discloses a kind of silicon-carbon cathode, preparation method, lithium ion battery and electric vehicles, are related to lithium ion battery silicon-carbon cathode technical field.Silicon-carbon cathode includes negative current collector and the coating for being set in turn in negative current collector surface and silicon-carbon cathode material layer；Coating includes: mesophase pitch, graphene and adhesive coating, and the mass ratio of mesophase pitch, graphene and binder is 20-50:40-65:1.5-10.Coating includes the coating of mesophase pitch, graphene and binder on silicon-carbon cathode collector of the invention, silicon-carbon cathode electric conductivity, thermal diffusivity can be improved, improve cycle performance, safety and the high current charge-discharge ability of lithium ion battery, the preferred water system PVDF of binder, it is cooperateed with negative electrode material binder water system PVDF, the cohesive force for enhancing coating and negative electrode material interlayer, further increases cycle performance.
Description
Technical field
The present invention relates to lithium ion battery silicon-carbon cathode technical fields, in particular to a kind of silicon-carbon cathode, its preparation
Method, lithium ion battery and electric vehicle.
Background technique
To negative electrode material, more stringent requirements are proposed for the raising of lithium ion battery energy density, and graphite cathode theory is held at present
The performance of amount is up to 95% or more, using having been approached its theoretical limit.Compared with graphite cathode, silicon based anode material energy is close
Spend with the obvious advantage, theoretical specific capacity may be up to 4200mAh/g, and due to the advantages such as its rich reserves, intercalation potential be low, become
The hot spot of negative electrode material research and application.
But there are many problems demands in practical applications and solve in silicon based anode material, be mainly shown as:
1, silicon bulk effect during embedding de- lithium is big, and high cubical expansivity makes silicon particle dusting in cyclic process
Seriously, capacity attenuation is rapid；
2, silicon is semiconductor, and electric conductivity is more far short of what is expected than graphite cathode, significantly impacts silicon substrate system lithium cell for the first time
Coulombic efficiency and high current charge-discharge ability.
Si-C composite material is as a kind of typical silicon based anode material, it may have the above problem.
It is therefore desired to provide a kind of silicon-carbon cathode, it is able to solve at least one of above problem.
In view of this, the present invention is specifically proposed.
Summary of the invention
One of the objects of the present invention is to provide a kind of silicon-carbon cathode, it is coated on negative current collector and is mainly dripped by interphase
The coating of green, graphene and adhesive coating composition, which can be improved silicon-carbon cathode electric conductivity and thermal diffusivity, to improve lithium
Cycle performance, safety and the high current charge-discharge ability of ion battery.
The second object of the present invention is to provide a kind of preparation method of above-mentioned silicon-carbon cathode, by coating material and cathode material
Material is made slurry and is coated, easy to operate, easy to produce.
The third object of the present invention is to provide a kind of lithium ion battery, including above-mentioned silicon-carbon cathode or above-mentioned silicon-carbon cathode
The silicon-carbon cathode that is prepared of preparation method.
The fourth object of the present invention is a kind of electric vehicle, including above-mentioned lithium ion battery.
In order to realize above-mentioned purpose of the invention, the following technical scheme is adopted:
In a first aspect, provide a kind of silicon-carbon cathode, including negative current collector and it is set in turn in the negative pole currect collecting
The coating and silicon-carbon cathode material layer in body surface face；
The coating includes mesophase pitch, graphene and adhesive coating, the mesophase pitch, the graphene and
The mass ratio of the adhesive coating is 20-50:40-65:1.5-10.
Preferably, on the basis of technical solution provided by the invention, the mesophase pitch, the graphene and described
The mass ratio of adhesive coating is 30-40:45-55:2-8；
Preferably, the mass ratio of the mesophase pitch, the graphene and the adhesive coating is 30-35:50-
55:3-6。
Preferably, on the basis of technical solution provided by the invention, the silicon-carbon cathode material layer includes: silicon-carbon cathode
Active material, conductive agent and negative electrode material binder, the conductive agent include conductive black and single-walled carbon nanotube, the conduction
Carbon black and the single-walled carbon nanotube mass ratio are 1-20:1, preferably 5-15:1.
Preferably, on the basis of technical solution provided by the invention, the adhesive coating and the negative electrode material are viscous
Tying agent independently includes water system PVDF.
Preferably, on the basis of technical solution provided by the invention, the silicon-carbon cathode active material is sub- using oxidation
Silicon is combined with graphite, wherein aoxidizing sub- silicon and accounting for the mass ratio of silicon-carbon cathode active material is 5-25%.
Preferably, on the basis of technical solution provided by the invention, silicon-carbon cathode active material, conductive agent and cathode material
The mass ratio for expecting binder is 70-99.5:0.1-15:0.1-15.
Second aspect provides a kind of preparation method of above-mentioned silicon-carbon cathode, comprising the following steps:
The first applying coating slurry on negative current collector, is coated with silicon-carbon cathode material slurry after dry, it is negative to obtain silicon-carbon
Pole；
Coating paste is obtained by the way that mesophase pitch, graphene and adhesive coating to be dissolved or dispersed in solvent；Silicon
Carbon negative pole material slurry is by the way that silicon-carbon cathode active material, conductive agent and negative electrode material binder to be dissolved or dispersed in solvent
It obtains.
Preferably, on the basis of technical solution provided by the invention, the preparation method of silicon-carbon cathode, including following step
It is rapid:
(a) coating paste and negative electrode material slurry are provided: in mass ratio by mesophase pitch, graphene and water system PVDF
20-50:40-65:1.5-10 being dissolved or dispersed in solvent, coating paste is obtained；By silicon-carbon cathode active material, conductive agent and
Water system PVDF 70-99.5:0.1-15:0.1-15 in mass ratio is dissolved or dispersed in solvent, obtains negative electrode material slurry；It is conductive
Agent is the combination of conductive black and single-walled carbon nanotube, and conductive black and single-walled carbon nanotube mass ratio are 1-20:1；
(b) first coating paste is coated uniformly on negative current collector, dries and removes solvent, form coating, then by cathode
Material paste is coated in and has been coated on cated negative current collector, dries and removes solvent, obtains silicon-carbon cathode.
The third aspect provides a kind of lithium ion battery, the preparation side including above-mentioned silicon-carbon cathode or above-mentioned silicon-carbon cathode
The silicon-carbon cathode that method is prepared.
Fourth aspect provides a kind of electric vehicle, including above-mentioned lithium ion battery.
Compared with the prior art, the invention has the following beneficial effects:
(1) lithium ion battery silicon-carbon cathode collector of the present invention is equipped with coating, and the coating is mainly by a certain proportion of painting
Layer binder, mesophase pitch and graphene composition, melt asphalt phase as carbon material, can be completely infused in graphene gap
And in current collector foil, melts asphalt phase and graphene collaboration increases the conductive capability of silicon-carbon cathode；Stone can also be played simultaneously
The black good heat-sinking capability of alkene, improves the heat-sinking capability of collector.The high conductivity coating improves silicon-carbon cathode lithium battery
Cycle performance, safety and high current charge-discharge ability.
In addition, conductive agent preferably uses conductive black to receive with single wall carbon in lithium ion battery silicon-carbon cathode material system
The mode of mitron Joint of Line and Dot can construct good conductive network in the electrodes, play high-rate characteristics；Wherein SWCNT is good
Heating conduction be conducive to heat dissipation when battery charging and discharging, reduce the polarization of battery, improve the high temperature performance of battery, extend battery
Service life；In addition, the preferred water system PVDF of binder, can play synergistic effect, Ke Yiyong with negative electrode material binder water system PVDF
To enhance the electronic contact between electrode active material and conductive agent and active material and collector, collaboration CNT threadiness network
The effect of structure, can preferably stable pole piece structure, better buffer function is played to the volume expansion of silicon-carbon cathode, into one
Walk the cyclicity for improving lithium ion battery and big multiplying power discharging property.
(2) coating material and negative electrode material are made slurry and coated by the preparation method of silicon-carbon cathode of the present invention, operation
Simply, easy to produce.
Detailed description of the invention
Fig. 1 is the charge and discharge cycles test result figure at 25 DEG C of the lithium ion battery progress that embodiment and comparative example obtains.
Specific embodiment
Embodiment of the present invention is described in detail below in conjunction with embodiment, but those skilled in the art will
Understand, the following example is merely to illustrate the present invention, and is not construed as limiting the scope of the invention.It is not specified in embodiment specific
Condition person carries out according to conventional conditions or manufacturer's recommended conditions.Reagents or instruments used without specified manufacturer is
The conventional products that can be obtained by commercially available purchase.
According to an aspect of the invention, there is provided a kind of silicon-carbon cathode, including negative current collector and it is set in turn in
The coating and silicon-carbon cathode material layer on negative current collector surface；Coating is mainly by mesophase pitch, graphene and adhesive coating
Composition, the mass ratio of mesophase pitch, graphene and adhesive coating are 20-50:40-65:1.5-10；Silicon-carbon cathode material layer
Mainly it is made of silicon-carbon cathode active material, conductive agent and negative electrode material binder.
Typical but non-limiting negative current collector can be for example copper foil, and the thickness of negative current collector is preferably 5-30 μ
m。
Coating is coated on negative current collector, the composition of coating includes mesophase pitch, graphene and adhesive coating, in
Between asphalt phase, graphene and binder mass ratio be 20-50:40-65:1.5-10.
It can effectively reduce the internal resistance of cell on graphene coating negative current collector, improve electric conductivity and thermal diffusivity.
Mesophase pitch (also known as intermediate melt asphalt phase, mesophase pitch, abbreviation MP) is one kind by average molecular
The mixture for a variety of flat plate-like condensed-nuclei aromatics compositions that quality is 370~2000, is called liquid crystal asphalt phase.If general substance is with crystalline substance
Body state, which exists, is then presented optical anisotropy, exists with liquid condition and optical isotropy is then presented；But there is a substance
It is being the intermediate stage of liquid process (or inverse process) from crystalline transformation, is showing a kind of optically anisotropic turbidity fluid shape
State is both that liquid form has crystal optics anisotropic character again simultaneously, is referred to as liquid crystal in crystallography, object mutually learn in then claim
Be interphase.
Adhesive coating plays cementation, and typical but non-limiting adhesive coating is, for example, water system Kynoar
(PVDF)。
The typical but non-limiting mass ratio of mesophase pitch, graphene and binder is, for example, 20:40:1.5,20:
65:5,20:60:10,30:65:5,30:40:1.5,30:60:10,40:40:1.5,50:65:5 or 50:60:10 etc..
By using mesophase pitch, to graphene and current collector foil thorough impregnation, is formed and coat C, mesophase pitch,
Graphene and binder play high conductivity, high-cooling property with the coating that certain proportion is formed.
Silicon-carbon cathode material layer is formed by silicon-carbon cathode material, including silicon-carbon cathode active material, conductive agent and negative
Pole material binder.
Silicon-carbon cathode active material is that the carbon material of different shape carrys out the composite material that compound silicon materials are formed, to carbon material
It is not construed as limiting with source, the type of silicon materials etc..Typical but non-limiting silicon materials are, for example, nano-silicon, silica, oxidation
Sub- silicon or silicon-containing alloy etc., carbon material it is typical but non-limiting be, for example, hard carbon, soft carbon, natural graphite, artificial graphite or in
Between phase carbosphere etc..
The content of carbon material and silicon materials is not construed as limiting, the mass ratio of typical but non-limiting silicon materials and carbon material
It such as can be 1:0.1-100.
Conductive agent is not construed as limiting, can using well known to a person skilled in the art cathode conductive agent, conductive agent it is typical but
Unrestricted is, for example, carbon nanotube (CNT), graphene, electrically conductive graphite, conductive carbon black, Ketjen black ECP or carbon fiber
(VGCF) one or more of in.
The type of negative electrode material binder is not construed as limiting, typical but non-limiting negative electrode material binder is, for example, poly-
Acrylic acid (PAA), polyvinyl alcohol (PVA), sodium carboxymethylcellulose (CMC), butadiene-styrene rubber (SBR), sodium alginate (ALG), fluorine
Change one or more of rubber, acrylonitrile multiple copolymer (LA system) or water system Kynoar (PVDF).
Lithium ion battery silicon-carbon cathode collector of the present invention is equipped with coating, and the coating is mainly by a certain proportion of bonding
Agent, mesophase pitch and graphene composition, melt asphalt phase to graphene and current collector foil thorough impregnation, which can be improved
Silicon-carbon cathode electric conductivity, and graphene can also give full play to its good thermal diffusivity, improve the heat-sinking capability of collector.It should
High conductivity coating improves cycle performance, safety and the high current charge-discharge ability of silicon-carbon cathode lithium battery.
Preferably, the mass ratio of mesophase pitch, graphene and adhesive coating is 30-40:45-55:2-8；
It is further preferred that the mass ratio of mesophase pitch, graphene and adhesive coating is 30-35:50-55:3-6.
By the ratio of optimization mesophase pitch, graphene and adhesive coating three, coating can be further increased
Electric conductivity forms the silicon-carbon cathode of more high conductivity and high-cooling property.
In a preferred embodiment, conductive agent includes conductive black and single-walled carbon nanotube, conductive black and list
Wall carbon nano tube mass ratio is 1-20:1, preferably 5-15:1.
Conductive black (SP) partial size is small, large specific surface area, is not construed as limiting to the type of conductive black, typical but non-limiting
Be, for example, acetylene black, Super P, Super S, 350G or Ketjen black etc..
Single-walled carbon nanotube (SWCNT) is crimped by single layer flake graphite, to the type and ruler of single-walled carbon nanotube
It is very little to be not construed as limiting, it can be unmodified single-walled carbon nanotube, be also possible to the single-walled carbon nanotube by modification.
The mass ratio of conductive black and single-walled carbon nanotube such as can for 1:1,2:1,3:1,4:1,5:1,6:1,7:1,
8:1,9:1,10:1,11:1,12:1,13:1,14:1,15:1,16:1,17:1,18:1,19:1 or 20:1.
It is used cooperatively by conductive black and single-walled carbon nanotube, is led so that forming point-line between silicon-carbon cathode particle
Electric network, establishes good conductive channel between silicon-carbon cathode particle, and line style single-walled carbon nanotube conductive agent can play
The effect for fettering electrode material expansion, reduces pole piece expansion rate, improves the stability of circulating battery.
In a preferred embodiment, adhesive coating and negative electrode material binder independently include water system
PVDF。
Negative electrode material binder water system PVDF and coating water system PVDF on a current collector act synergistically, so that coating and negative
The cohesive force of pole material interlayer, further improve lithium ion battery cyclicity and big multiplying power discharging property.
In a preferred embodiment, silicon-carbon cathode active material is combined using sub- silicon is aoxidized with graphite,
In, aoxidizing sub- silicon and accounting for the mass ratio of silicon-carbon cathode active material is 5-25%.
Aoxidize sub- silicon account for the mass fraction of silicon-carbon cathode active material include but is not limited to such as 5%, 10%, 15%,
20% or 25%.
It is preferred that the silicon-carbon cathode material being compounded to form using sub- silicon and graphite is aoxidized, by selecting carbon material and silicon materials,
The theoretical capacity for aoxidizing sub- silicon is lower than silicon, and graphite has greatly improved to the chemical property for aoxidizing sub- silicon, and it is sub- to adjust oxidation
Silicone content, material show higher specific capacity, low volume expansion and good electrochemical cycle stability.
In a preferred embodiment, the quality of silicon-carbon cathode active material, conductive agent and negative electrode material binder
Than for 70-99.5:0.1-15:0.1-15.
The mass ratio of silicon-carbon cathode active material, conductive agent and negative electrode material binder is typical but non-limiting to be, for example,
70:15:15,80:10:10,90:5:5 or 99.5:0.25:0.25 etc..
Conductive agent and binder in lithium ion battery negative material containing special ratios, activity when being conducive to make pole piece
Substance can be perfectly adhered on collector, improve the efficiency for charge-discharge of electrode.Conductive agent and binder content are adjusted, into one
Step improves the content of active material.
According to the second aspect of the invention, a kind of preparation method of above-mentioned silicon-carbon cathode is provided, comprising the following steps:
The first applying coating slurry on negative current collector, is coated with silicon-carbon cathode material slurry after dry, it is negative to obtain silicon-carbon
Pole；Coating paste is mainly dissolved or dispersed in solvent by the mesophase pitch of mass ratio, graphene and adhesive coating and is obtained；
Silicon-carbon cathode material slurry is mainly dissolved or dispersed in solvent by silicon-carbon cathode active material, conductive agent and negative electrode material binder
In obtain.
Description to the mesophase pitch of coating paste, graphene and adhesive coating and to silicon-carbon cathode material slurry
Silicon-carbon cathode active material, the description of conductive agent and negative electrode material binder it is identical as the corresponding description in first aspect,
This is repeated no more.
Preferred solvent is any one in water or N-Methyl pyrrolidone.
It is made slurry coating after slurry on a current collector, after solvent volatilization, coating material and silicon-carbon cathode material are fixed
In on negative current collector.
Preferably, the viscosity of coating paste and silicon-carbon cathode material slurry independently is 3000~7000mPas, glues
Degree can be by adjusting binder content de-regulation.
The mode of homogenate is not construed as limiting, is preferably homogenized by dry or wet technique, slurry is obtained, then uniformly coating
On negative current collector, drying mode is preferably dried, and obtains silicon-carbon cathode after carrying out roll-in, cross cutting after preferably drying.
Coating material and negative electrode material are made slurry and coated by the preparation method of silicon-carbon cathode of the present invention, operation letter
It is single, it is easy to produce.
Preferably, a kind of preparation method of typical silicon-carbon cathode, comprising the following steps:
(a) coating paste and negative electrode material slurry are provided: in mass ratio by mesophase pitch, graphene and water system PVDF
20-50:40-65:1.5-10 being dissolved or dispersed in solvent, coating paste is obtained；By silicon-carbon cathode active material, conductive agent and
Water system PVDF 70-99.5:0.1-15:0.1-15 in mass ratio is dissolved or dispersed in solvent, obtains negative electrode material slurry；Silicon-carbon
Negative electrode active material is combined using sub- silicon is aoxidized with graphite, and aoxidizing the mass ratio that sub- silicon accounts for silicon-carbon cathode active material is 5-
25%；Conductive agent is the combination of conductive black and single-walled carbon nanotube, and conductive black and single-walled carbon nanotube mass ratio are 1-20:
1；
(b) first coating paste is coated uniformly on negative current collector, dries and removes solvent, form coating, then by cathode
Material paste, which is coated uniformly on, to be had been coated on cated negative current collector, obtains silicon-carbon cathode after dry, roll-in and cross cutting.
According to the third aspect of the present invention, a kind of lithium ion battery, including above-mentioned silicon-carbon cathode or above-mentioned silicon are provided
The silicon-carbon cathode that the preparation method of Carbon anode is prepared.
Lithium ion battery includes the silicon-carbon that the preparation method of anode, above-mentioned silicon-carbon cathode or above-mentioned silicon-carbon cathode is prepared
Cathode, diaphragm and electrolyte.
The battery of various shapes that lithium ion battery can be well known to those skilled in the art, for example, can for it is round,
The battery of the shapes such as rectangular.
In conductive good, good cycle the effect of the silicon-carbon cathode of embodiment of the present invention, the present invention is being used
The lithium ion battery of the silicon-carbon cathode of embodiment can also obtain identical effect.
According to the fourth aspect of the present invention, a kind of electric vehicle, including above-mentioned lithium ion battery are provided.
Electric vehicle is the electric vehicle run as driving power by lithium ion battery, and can be in addition to lithium from
The automobile (including hybrid electric vehicle) of other driving sources is also equipped with except sub- battery.
Identical effect can also be obtained in the electric vehicle of the lithium ion battery using embodiment of the present invention.
In order to further appreciate that the present invention, combined with specific embodiments below with comparative example to the method for the present invention and effect do into
One step detailed description.The following example is merely to illustrate the present invention, and is not construed as limiting the scope of the invention.In embodiment
The person that is not specified actual conditions, carries out according to conventional conditions or manufacturer's recommended conditions.Production is not specified in agents useful for same or instrument
Manufacturer person is the conventional products that can be obtained by commercially available purchase.
Embodiment 1
A kind of silicon-carbon cathode including negative current collector copper foil and is set in turn in the coating of negative current collector copper foil surface
With silicon-carbon cathode material layer；
Coating is made of mesophase pitch, graphene and the water system Kynoar that mass ratio is 30:65:5；Silicon-carbon cathode
Material layer is made of silicon-carbon cathode active material, conductive agent and the negative electrode material binder that mass ratio is 95.4:1.1:3.5, silicon
Carbon anode active material is combined using SiO with graphite, SiO mass accounting 8%, and conductive agent is conductive black (SP), cathode
Material binder is the sodium carboxymethylcellulose and butadiene-styrene rubber that mass ratio is 4:3.
The preparation method of above-mentioned silicon-carbon cathode, comprising the following steps:
(1) by the mesophase pitch of quality accounting 30%, 65% graphene and 5% sodium carboxymethylcellulose with wet process
Slurry is made in technique, is evenly applied on negative current collector copper foil, is formed and has cated copper foil；
(2) by the silicon-carbon cathode material of quality accounting 95.4% (SiO mass accounting 8%), 1.1% conductive black
(SP), slurry is made with wet processing in 2% sodium carboxymethylcellulose and 1.5% butadiene-styrene rubber, is evenly applied to have painting
The copper foil surface of layer, drying, roll-in and cross cutting obtain silicon-carbon cathode.
Embodiment 2
A kind of silicon-carbon cathode including negative current collector copper foil and is set in turn in the coating of negative current collector copper foil surface
With silicon-carbon cathode material layer；
Coating is made of mesophase pitch, graphene and the water system Kynoar that mass ratio is 40:55:5；Silicon-carbon cathode
Material layer is made of silicon-carbon cathode active material, conductive agent and the negative electrode material binder that mass ratio is 95.4:1.1:3.5, silicon
Carbon anode active material is combined using SiO with graphite, SiO mass accounting 8%, and conductive agent is conductive black (SP), cathode
Material binder is the sodium carboxymethylcellulose and butadiene-styrene rubber that mass ratio is 3:4.
The preparation method of above-mentioned silicon-carbon cathode, comprising the following steps:
(1) by the mesophase pitch of quality accounting 40%, 45% graphene and 5% sodium carboxymethylcellulose with wet process
Slurry is made in technique, is evenly applied on negative current collector copper foil, is formed and has cated copper foil；
(2) by the silicon-carbon cathode material of quality accounting 95.4% (SiO mass accounting 8%), 1.1% conductive black
(SP), slurry is made with wet processing in 1.5% sodium carboxymethylcellulose and 2% butadiene-styrene rubber, is evenly applied to have painting
The copper foil surface of layer, drying, roll-in and cross cutting obtain silicon-carbon cathode.
Embodiment 3
A kind of silicon-carbon cathode including negative current collector copper foil and is set in turn in the coating of negative current collector copper foil surface
With silicon-carbon cathode material layer；
Coating is made of mesophase pitch, graphene and the water system Kynoar that mass ratio is 50:40:10；Silicon-carbon is negative
Pole material layer is made of silicon-carbon cathode active material, conductive agent and the negative electrode material binder that mass ratio is 95.5:1.5:3, silicon
Carbon anode active material is combined using SiO with graphite, SiO mass accounting 8%, and conductive agent is conductive black (SP), cathode
Material binder is the sodium carboxymethylcellulose and butadiene-styrene rubber that mass ratio is 4:3.
The preparation method of above-mentioned silicon-carbon cathode, comprising the following steps:
(1) by the mesophase pitch of quality accounting 50%, 40% graphene and 10% sodium carboxymethylcellulose with wet
Slurry is made in method technique, is evenly applied on negative current collector copper foil, is formed and has cated copper foil；
(2) by the silicon-carbon cathode material of quality accounting 95.5% (SiO mass accounting 8%), 1.5% conductive black
(SP), slurry is made with wet processing in 2% sodium carboxymethylcellulose and 1% butadiene-styrene rubber, is evenly applied to coating
Copper foil surface, drying, roll-in and cross cutting obtain silicon-carbon cathode.
Embodiment 4
The present embodiment the difference from embodiment 1 is that, butadiene-styrene rubber is replaced with into water system Kynoar.
Embodiment 5
The present embodiment the difference from embodiment 1 is that, conductive agent is the conductive black (SP) and single wall that mass ratio is 1:0.1
Carbon nanotube.The conductive black (SP) of corresponding preparation method 1.1% also replaces with 1% conductive black (SP) and 0.1%
Single-walled carbon nanotube.
Embodiment 6
The present embodiment the difference from embodiment 1 is that, conductive agent is the conductive black (SP) and multi wall that mass ratio is 1:0.1
Carbon nanotube.The conductive black (SP) of corresponding preparation method 1.1% also replaces with 1% conductive black (SP) and 0.1%
Multi-walled carbon nanotube.
Comparative example 1
A kind of silicon-carbon cathode including negative current collector copper foil and is set in turn in the silicon-carbon of negative current collector copper foil surface
Negative electrode material layer；
Silicon-carbon cathode active material, conductive agent and the cathode material that silicon-carbon cathode material layer is 95.4:1.1:3.5 by mass ratio
Expect that binder composition, silicon-carbon cathode active material are combined using SiO with graphite, SiO mass accounting 8%, conductive agent is to lead
Electric carbon black (SP), negative electrode material binder are the sodium carboxymethylcellulose and butadiene-styrene rubber that mass ratio is 4:3.
The preparation method of above-mentioned silicon-carbon cathode, comprising the following steps:
By the silicon-carbon cathode material (SiO mass accounting 8%) of quality accounting 95.4%, 1.1% conductive black (SP),
Slurry is made with wet processing in 2% sodium carboxymethylcellulose and 1.5% butadiene-styrene rubber, is evenly applied to copper foil surface, warp
Drying, roll-in and cross cutting obtain silicon-carbon cathode.
Comparative example 2
This comparative example the difference from embodiment 1 is that, mesophase pitch is replaced with to the graphene of equivalent.
Test example
By nickle cobalt lithium manganate tertiary cathode material, carbon nanotube and the Kynoar of high nickel content (75%) according to 97:
The mass ratio of 1:2, which is dispersed in N-Methyl pyrrolidone, obtains anode sizing agent, and anode sizing agent is coated on plus plate current-collecting body aluminium foil
Surface, obtain positive plate by drying, roll-in, cross cutting.
Negative electrode tab, electrolyte and the monolayer polyethylene that positive plate is obtained with embodiment 1-6 and comparative example 1-2 respectively
(PE) lithium ion battery is respectively prepared with lamination process in diaphragm, is tested.
Test 1
The lithium ion battery that embodiment 1-6 and comparative example 1-2 are obtained carries out 1C/2C/3C/5C discharge test, voltage
Range 4.2-3.0V, the results are shown in Table 1.
Table 1
Test 2
The lithium ion battery that embodiment and comparative example is obtained carries out the charge and discharge cycles test at 25 DEG C, and voltage range is
4.2-3.0V as a result as shown in Figure 1.
By test 1 and test 2 as can be seen that the present invention under silicon-carbon cathode system on negative current collector by being arranged
Coating including mesophase pitch, graphene and binder, it is complete to graphene and current collector foil which melts asphalt phase
Dipping can significantly improve the electric conductivity of silicon-carbon cathode, and graphene can also give full play to its good thermal diffusivity, improve collector
Heat-sinking capability.The high conductivity coating improve silicon-carbon cathode lithium ion battery circulation and big multiplying power discharging property.
Comparative example 1 compared with Example 1, uncoated coating on negative current collector, the big multiplying power discharging of lithium ion battery
Performance is decreased obviously.Comparative example 2 compared with Example 1, does not contain mesophase pitch, during the electric conductivity of coating is not so good as in coating
Between the asphalt phase coating that is collectively constituted with graphene conduct electricity very well, the circulation of lithium ion battery and big multiplying power discharging property are not
Ideal effect can be reached.
Further analysis, when 4 adhesive coating of embodiment selects water system PVDF, performance is better than the combination of CMC and SBR,
Speculate the reason for this is that: water system PVDF binder and coating water system PVDF on a current collector act synergistically, and further improve lithium
The cyclicity of ion battery and big multiplying power discharging property.
The silicon-carbon cathode material conductive agent of embodiment 5 is used in combination using conductive black with single-walled carbon nanotube, embodiment 5
Cycle performance of lithium ion battery and high rate charge-discharge performance when being superior to electrically conductive graphite and playing a role separately as conductive agent
Performance, it can thus be seen that further pressing down when electrically conductive graphite (SP) and single-walled carbon nanotube (SWCNT) Joint of Line and Dot act on
The expansion for having made electrode improves the cycle performance of battery.And electrically conductive graphite (SP) and multi-walled carbon nanotube (SWCNT) is used to tie
It closes the effect used and is not so good as the effect being used in combination using electrically conductive graphite (SP) with single-walled carbon nanotube (SWCNT), this is because,
The dispersion effect of multi-walled carbon nanotube is much less than single-walled carbon nanotube, poor with silicon-carbon cathode material Combination, and formation is led
Electric network smoothness is poor, to affect the performance of carbon nanotube effect.
Although illustrate and describing the present invention with specific embodiment, it will be appreciated that without departing substantially from of the invention
Many other change and modification can be made in the case where spirit and scope.It is, therefore, intended that in the following claims
Including belonging to all such changes and modifications in the scope of the invention.
Claims (10)
1. a kind of silicon-carbon cathode, which is characterized in that including negative current collector and be set in turn in the negative current collector surface
Coating and silicon-carbon cathode material layer；
The coating includes: mesophase pitch, graphene and adhesive coating, the mesophase pitch, the graphene and institute
The mass ratio for stating adhesive coating is 20-50:40-65:1.5-10.
2. silicon-carbon cathode according to claim 1, which is characterized in that the mesophase pitch, the graphene and described
The mass ratio of adhesive coating is 30-40:45-55:2-8；
Preferably, the mass ratio of the mesophase pitch, the graphene and the adhesive coating is 30-35:50-55:3-
6。
3. silicon-carbon cathode according to claim 1, which is characterized in that the silicon-carbon cathode material layer includes: silicon-carbon cathode
Active material, conductive agent and negative electrode material binder；Wherein,
The conductive agent includes conductive black and single-walled carbon nanotube, the conductive black and the single-walled carbon nanotube mass ratio
For 1-20:1, preferably 5-15:1.
4. silicon-carbon cathode according to claim 3, which is characterized in that the adhesive coating and negative electrode material bonding
Agent independently includes water system PVDF.
5. silicon-carbon cathode according to claim 3, which is characterized in that the silicon-carbon cathode active material is using the sub- silicon of oxidation
It is combined with graphite, wherein aoxidizing sub- silicon and accounting for the mass ratio of silicon-carbon cathode active material is 5-25%.
6. silicon-carbon cathode according to claim 3, which is characterized in that silicon-carbon cathode active material, conductive agent and cathode material
The mass ratio for expecting binder is 70-99.5:0.1-15:0.1-15.
7. a kind of preparation method of silicon-carbon cathode, which comprises the following steps:
The first applying coating slurry on negative current collector, is coated with silicon-carbon cathode material slurry after dry, obtains silicon-carbon cathode；
Coating paste is obtained by the way that mesophase pitch, graphene and adhesive coating to be dissolved or dispersed in solvent；Silicon-carbon is negative
Pole material paste is obtained by the way that silicon-carbon cathode active material, conductive agent and negative electrode material binder to be dissolved or dispersed in solvent
It arrives.
8. the preparation method of silicon-carbon cathode according to claim 7, which comprises the following steps:
(a) coating paste and negative electrode material slurry are provided: by mesophase pitch, graphene and water system PVDF 20-50 in mass ratio:
40-65:1.5-10 is dissolved or dispersed in solvent, obtains coating paste；By silicon-carbon cathode active material, conductive agent and water system
PVDF 70-99.5:0.1-15:0.1-15 in mass ratio is dissolved or dispersed in solvent, obtains negative electrode material slurry；Conductive agent is
The combination of conductive black and single-walled carbon nanotube, conductive black and single-walled carbon nanotube mass ratio are 1-20:1；
(b) first coating paste is coated uniformly on negative current collector, dries and removes solvent, form coating, then by negative electrode material
Slurry is coated in and has been coated on cated negative current collector, dries and removes solvent, obtains silicon-carbon cathode.
9. a kind of lithium ion battery, which is characterized in that including silicon-carbon cathode described in any one of claims 1-6 or according to right
It is required that the silicon-carbon cathode that the preparation method of silicon-carbon cathode described in 7 or 8 obtains.
10. a kind of electric vehicle, which is characterized in that including lithium ion battery as claimed in claim 9.
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