CN102916161A - Electrode composite material for lithium ion battery and preparation method thereof - Google Patents
Electrode composite material for lithium ion battery and preparation method thereof Download PDFInfo
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- CN102916161A CN102916161A CN2012102692243A CN201210269224A CN102916161A CN 102916161 A CN102916161 A CN 102916161A CN 2012102692243 A CN2012102692243 A CN 2012102692243A CN 201210269224 A CN201210269224 A CN 201210269224A CN 102916161 A CN102916161 A CN 102916161A
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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 discloses an electrode composite material for a lithium ion battery and a preparation method thereof. The electrode composite material comprises a current collector, an electrode material, a carbonized medium and a porosity polymer adhesive; the current collector adopts metal foam with a plurality of penetration holes; the electrode material is filled in a plurality of penetration holes of the current collector; the carbonized medium is positioned between the current collector and the electrode material; and the porosity polymer adhesive is positioned on the surface of the current collector. The preparation method comprises the following steps of: mixing an adhesive, the electrode material and a conductive additive; filling the mixture into a plurality of penetration holes of the current collector; and drying, die-casting and calcining, coating the porosity polymer adhesive on the surface of the current collector after cooling, and drying to obtain the electrode composite material. According to the electrode composite material for the lithium ion battery and the preparation method thereof, which are provided by the invention, the circulating stability is improved, the electrode composite material has a good mechanical performance and a good bending resistance, the stripping phenomenon of the electrode material is effectively retarded and the performance and the service life of the battery are greatly improved.
Description
Technical field
The present invention relates to novel energy material technology field, particularly relate to electrode composite material of a kind of lithium ion battery and preparation method thereof.
Background technology
The preparation method of the electrode composite material of lithium ion battery is coated in electrode material on the tinsel and is shaped by adhesive to obtain traditionally, the shortcoming of the method has in coating procedure can use more adhesive, cause the partial electrode material not take full advantage of, can't obtain the electrode composite material of high areal density, adhesion between electrode material and the collector is relatively poor simultaneously, easily produce the electrode peeling phenomenon, reduce its Mechanical Reliability, the rate of curving is limited.Electrode composite material is applied in the battery product, the capacitance of battery product is reduced, internal resistance increases, shorten useful life, processing technology complexity and cost increase, and has limited the extensive use of lithium battery.
Usually adopt tinsel as collector, in cyclic process, electrode material is along with the embedding of lithium ion and take off the Swelling and contraction of embedding meeting generation volume, the mechanical stress that produces makes electrode material gradually efflorescence in cyclic process, the cracking that causes electrode and collector with peel off, electrically contact forfeiture between the active material, internal resistance increases, and shows relatively poor charge-discharge performance.For fear of this technical problem, it is relatively thin that existing electrode composite material need to be made, cause the surface density of electrode material less, and in order to obtain corresponding capacity and energy density, need to adopt thicker coating and a large amount of multi-disc laminated in the follow-up battery assembling processing, when coating layer thickness is larger, can make again the poor processability of electrode, being accumulated in of this multilayer also can cause the internal resistance of cell to increase and the decline of stable circulation performance on the performance.Existence than thick coating also makes the electrode material frangibility, and itself and collector are separated.Even adopt thinner electrode composite material, can't realize that also less curvature changes, and has limited structure and the profile of the battery products such as curled battery.Mutual restriction on these prior aries has caused the parameters such as internal resistance, life-span and the energy density of battery of the prior art and capacity can't obtain the improvement of essence.
Summary of the invention
The technical problem that the present invention mainly solves provides a kind of electrode composite material that makes the lithium ion battery that battery performance is better, the life-span is longer and preparation method thereof.
For solving the problems of the technologies described above, the technical scheme that the present invention adopts is: the electrode composite material that a kind of lithium ion battery is provided, comprise collector, electrode material, carbonization medium and porous polymer glue, described collector adopts the metal foam of many seepage holes, described electrode material is filled in many seepage holes of described collector, described carbonization medium is between described collector and described electrode material, and described porous polymer glue is positioned at the surface of described collector.
In a preferred embodiment of the present invention, the porosity of many seepage holes of described Collective Flow is 30%-95%, and the metal material of described metal foam comprises nickel, silver, gold, copper, aluminium and their alloy, stainless steel.
In a preferred embodiment of the present invention, described electrode material comprises positive electrode or negative material, and described positive electrode adopts the lithium ion compound, and described lithium ion compound comprises LiMn
2O
4, Li
3V
2(PO4)
3, LiFeM
1PO
4, LiMnO
2, LiMnM
2O
2, LiFePO
4In one or more, M wherein
1Comprise Ni, Co, Mn, Mg, Ca, Cr, V, Sr, M
2Comprise Ni, Co, Mg, Ca, Cr, V, Sr, described negative material comprises material with carbon element, silicon materials, SiO
2, nitride, SnO
2, Sb
2O
3, Li
4Ti
5O
12In one or more, described material with carbon element comprises natural or artificial synthetic graphite, celion, carbonaceous mesophase spherules, hard carbon, carbon nano-tube, Graphene.
In a preferred embodiment of the present invention, described carbonization medium is space network, coats described collector and described electrode material.
In a preferred embodiment of the present invention, described porous polymer glue comprises polyvinylidene fluoride, polytetrafluoroethylene, polyoxyethylene, polymethyl acrylate, have in the polymer of acrylate monomer one or more, the thickness of described porous polymer glue is 1 μ m-5 μ m, and viscosity is 0.1PaS-10PaS.
In a preferred embodiment of the present invention, described electrode composite material is flaky material, and thickness is 100 μ m-100cm.
Preparation method's step of the electrode composite material of described lithium ion battery is: add adhesive and make colloidal solution in solvent, add again electrode material and conductive agent, be stirred into the paste slurry, the slurry that obtains is filled in many seepage holes of collector, carries out the drying first time, be cast into certain thickness with Pressing device, in inert gas, calcine again, apply porous polymer glue at collection liquid surface after the cooling, carry out the drying second time, obtain the electrode composite material of lithium ion battery.
In a preferred embodiment of the present invention, described adhesive comprises one or more in polyethylene, polypropylene, polybutadiene, sodium carboxymethylcellulose, polyvinylidene fluoride, polytetrafluoroethylene, polyacrylonitrile, ethylene propylene diene rubber, synthetic rubber, the polyurethane, and described conductive agent comprises carbon black, acetylene black, carbon nano-tube, ultra-fine carbon dust or gas-phase growth of carbon fibre.
In a preferred embodiment of the present invention, dry and the described second time of the described first time, the temperature of drying was 90 ℃-110 ℃, the dry time is 4h-12h for the first time, and the dry time is 1h-10h for the second time, and described calcination process is to carry out 2h-8h under 500 ℃-1200 ℃.
The invention has the beneficial effects as follows: electrode composite material of lithium ion battery of the present invention and preparation method thereof, effectively alleviated the mechanical stress effect that produces because of bulk effect in the charge and discharge process, improved cyclical stability, possess preferably mechanical performance and resistant to bending performance, effectively slowed down the peeling of electrode material, be applied in the lithium battery, make battery product that larger battery capacity be arranged, the substance that has guaranteed battery internal resistance in the charge and discharge cycles process reduces, and makes battery performance and life-span all obtain good assurance.
Embodiment
The below is described in detail preferred embodiment of the present invention, thereby so that advantages and features of the invention can be easier to be it will be appreciated by those skilled in the art that protection scope of the present invention is made more explicit defining.
The invention provides a kind of electrode composite material of lithium ion battery, comprise collector, electrode material, carbonization medium and porous polymer glue, described collector adopts the metal foam of many seepage holes, described electrode material is filled in many seepage holes of described collector, described carbonization medium is between described collector and described electrode material, and described porous polymer glue is positioned at the surface of described collector.
The porosity of many seepage holes of wherein said Collective Flow is 30%-95%, and the metal material of described metal foam comprises nickel, silver, gold, copper, aluminium and their alloy, stainless steel.Described electrode material comprises positive electrode or negative material, and described positive electrode adopts the lithium ion compound, and described lithium ion compound comprises LiMn
2O
4, Li
3V
2(PO4)
3, LiFeM
1PO
4, LiMnO
2, LiMnM
2O
2, LiFePO
4In one or more, M wherein
1Comprise Ni, Co, Mn, Mg, Ca, Cr, V, Sr, M
2Comprise Ni, Co, Mg, Ca, Cr, V, Sr, described negative material comprises material with carbon element, silicon materials, SiO
2, nitride, SnO
2, Sb
2O
3, Li
4Ti
5O
12In one or more, described material with carbon element comprises natural or artificial synthetic graphite, celion, carbonaceous mesophase spherules, hard carbon, carbon nano-tube, Graphene.Described carbonization medium is space network, coats described collector and described electrode material.Described porous polymer glue comprises polyvinylidene fluoride, polytetrafluoroethylene, polyoxyethylene, polymethyl acrylate, comprise in the polymer of acrylate monomer one or more, the thickness of described porous polymer glue is 1 μ m-5 μ m, and viscosity is 0.1PaS-10PaS.Described electrode composite material can be flaky material, and thickness is 100 μ m-100cm.
Among the present invention, the preparation method's of the electrode composite material of described lithium ion battery embodiment comprises:
Embodiment one:
7g polyvinylidene fluoride adhesive is dissolved in the 180g 1-METHYLPYRROLIDONE, and fully stirring and dissolving is made colloidal solution, adds 140g LiFePO again
4With the ultra-fine carbon dust of 2.8g in colloidal solution, stir with mixer and to make the anode sizing agent of paste.Adopt slurry-scraping method that the anode sizing agent that obtains is filled in many seepage holes that porosity is 90% collector, wherein metal foam adopts aluminum, and it is 110 ℃ baking oven inner drying 4h that the collector of filling positive electrode is put into temperature.Taking out and using Pressing device die casting, thickness is 300 μ m, and wherein the size of thickness is decided according to the size of battery.With the 700 ℃ of lower calcining 2h in nitrogen of the material after the die casting, cool to room temperature takes out, and obtains the carbonization medium between positive electrode and collector.Applying one deck viscosity at collection liquid surface is the porousness polyvinylidene fluoride glue of 1PaS, puts into temperature and be 100 ℃ baking oven inner drying 2h, obtains anode composite material, and the positive electrode pole piece face specific capacity of gained anode composite material is approximately 40 mAh/cm
2, be higher than conventional value 12 mAh/cm far away
2
Embodiment two:
7g polyvinylidene fluoride adhesive is dissolved in the 180g 1-METHYLPYRROLIDONE, and fully stirring and dissolving is made colloidal solution, and the atomic ratio that adds again Li:Fe is that the gross mass of 1:2 is the Li of 180g
2CO
3And FePO
4, with the ultra-fine carbon dust of 2.5g in absolute ethyl alcohol, grind and to join in the colloidal solution after 4h fully mixes, stir with mixer and make the anode sizing agent of paste.Adopt slurry-scraping method that the anode sizing agent that obtains is filled in many seepage holes that porosity is 90% collector, wherein metal foam adopts aluminum, and it is 110 ℃ baking oven inner drying 4h that the collector of filling positive electrode is put into temperature.Taking out and using Pressing device die casting, thickness is 300 μ m, and wherein the size of thickness is decided according to the size of battery.With the 750 ℃ of lower calcining 3h in nitrogen of the material after the die casting, cool to room temperature takes out, and obtains the carbonization medium between positive electrode and collector.Applying one deck viscosity at collection liquid surface is the polyvinylidene fluoride glue of 1PaS, puts into temperature and be 100 ℃ baking oven inner drying 2h, obtains anode composite material.
Embodiment three:
7g polyvinylidene fluoride adhesive is dissolved in the 180g 1-METHYLPYRROLIDONE, and fully stirring and dissolving is made colloidal solution, and the atomic ratio that adds again Li:Mn:C is that the gross mass of 1:2:1 is the Li of 180g
2CO
3, MnO
2And glucose, grind 4h with the ultra-fine carbon dust of 2., 5 g, join in the colloidal solution after fully mixing, stir with mixer and make the anode sizing agent of paste.Adopt slurry-scraping method that the anode sizing agent that obtains is filled in many seepage holes that porosity is 90% collector, wherein metal foam adopts aluminum, and it is 110 ℃ baking oven inner drying 4h that the collector of filling positive electrode is put into temperature.Taking out and using Pressing device die casting, thickness is 300 μ m, and wherein the size of thickness is decided according to the size of battery.With the 350 ℃ of lower calcining 2h in nitrogen of the material after the die casting, at 700 ℃ of lower calcining 2h, cool to room temperature takes out, and obtains the carbonization medium between positive electrode and collector again.Applying one deck viscosity at collection liquid surface is the polyvinylidene fluoride glue of 1PaS, puts into temperature and be 100 ℃ baking oven inner drying 2h, obtains anode composite material.
Embodiment four:
7g polyvinylidene fluoride adhesive is dissolved in the 180g 1-METHYLPYRROLIDONE, and fully stirring and dissolving is made colloidal solution, adds 70g Li again
4Ti
5O
12With the ultra-fine carbon dust of 1.4g in colloidal solution, stir with mixer and to make the cathode size of paste.Adopt slurry-scraping method that the cathode size that obtains is filled in many seepage holes that porosity is 90% collector, wherein metal foam adopts copper product, and it is 110 ℃ baking oven inner drying 4h that the collector of filling negative material is put into temperature.Taking out and using Pressing device die casting, thickness is 150 μ m, and wherein the size of thickness is decided according to the size of battery.With the 650 ℃ of lower calcining 3h in nitrogen of the material after the die casting, cool to room temperature takes out, and obtains the carbonization medium between negative material and collector.Applying one deck viscosity at collection liquid surface is the polyvinylidene fluoride glue of 1PaS, puts into temperature and be 100 ℃ baking oven inner drying 2h, obtains anode material, and the positive electrode pole piece face specific capacity of gained anode composite material is approximately 44 mAh/cm
2, be higher than conventional value 13.2 mAh/cm far away
2
Embodiment five:
7g polyvinylidene fluoride adhesive is dissolved in the 180g 1-METHYLPYRROLIDONE, and fully stirring and dissolving is made colloidal solution, adds 60g SiO again
2, 10g carbon nano-tube and the ultra-fine carbon dust of 1.4g in colloidal solution, stir with mixer and to make the cathode size of paste.Adopt slurry-scraping method that the cathode size that obtains is filled in many seepage holes that porosity is 90% collector, wherein metal foam adopts copper product, and it is 110 ℃ baking oven inner drying 4h that the collector of filling negative material is put into temperature.Taking out and using Pressing device die casting, thickness is 150 μ m, and wherein the size of thickness is decided according to the size of battery.With the 650 ℃ of lower calcining 3h in nitrogen of the material after the die casting, cool to room temperature takes out, and obtains the carbonization medium between negative material and collector.Applying one deck viscosity at collection liquid surface is the polyvinylidene fluoride glue of 1PaS, puts into temperature and be 100 ℃ baking oven inner drying 2h, obtains anode material.
Embodiment six:
7g polyvinylidene fluoride adhesive is dissolved in the 180g 1-METHYLPYRROLIDONE, and fully stirring and dissolving is made colloidal solution, and the atomic ratio that adds again Li:Ti is that the gross mass of 4:5 is the Li of 110g
2CO
3And TiO
2, with the ultra-fine carbon dust of 1.8g in absolute ethyl alcohol, grind and to join in the colloidal solution after 4h fully mixes, stir with mixer and make the cathode size of paste.Adopt slurry-scraping method that the cathode size that obtains is filled in many seepage holes that porosity is 90% collector, wherein metal foam adopts copper product, and it is 110 ℃ baking oven inner drying 4h that the collector of filling negative material is put into temperature.Taking out and using Pressing device die casting, thickness is 150 μ m, and wherein the size of thickness is decided according to the size of battery.With the 700 ℃ of lower calcining 4h in nitrogen of the material after the die casting, cool to room temperature takes out, and obtains the carbonization medium between negative material and collector.Applying one deck viscosity at collection liquid surface is the polyvinylidene fluoride glue of 1PaS, puts into temperature and be 100 ℃ baking oven inner drying 2h, obtains anode material.
The beneficial effect of electrode composite material of the lithium ion battery that the present invention discloses and preparation method thereof is: (1) described collector is by having realized solid netted combination between many seepage holes skeleton and the electrode material, be nano level distance relation between the carbonization medium that in calcination process, produces and electrode material and the collector, the three has obtained sufficient contact, effectively alleviated the mechanical stress effect that produces because of bulk effect in the charge and discharge process, strengthen the stability between electrode material and the collector, improved cyclical stability; (2) application of die-casting technique can obtain the electrode composite material of multi-thickness sheet, and larger battery capacity is arranged, and possesses preferably mechanical performance and resistant to bending performance, satisfies the needs of different battery products; (3) the solid netted combination of the active material in the electrode material and collector, realized the superior electrical conductivity in the nanometer range, more stable interface is provided, effectively slowed down the peeling of electrode material, the substance that has guaranteed battery internal resistance in the charge and discharge cycles process reduces, avoided the battery performance decline phenomenon that therefore causes, battery performance and life-span have all obtained good assurance.
The above only is embodiments of the invention; be not so limit claim of the present invention; every equivalent structure or equivalent flow process conversion that utilizes description of the present invention to do; or directly or indirectly be used in other relevant technical fields, all in like manner be included in the scope of patent protection of the present invention.
Claims (9)
1. the electrode composite material of a lithium ion battery, it is characterized in that, comprise collector, electrode material, carbonization medium and porous polymer glue, described collector adopts the metal foam of many seepage holes, described electrode material is filled in many seepage holes of described collector, described carbonization medium is between described collector and described electrode material, and described porous polymer glue is positioned at the surface of described collector.
2. the electrode composite material of lithium ion battery according to claim 1 is characterized in that, the porosity of many seepage holes of described Collective Flow is 30%-95%, and the metal material of described metal foam comprises nickel, silver, gold, copper, aluminium and their alloy, stainless steel.
3. the electrode composite material of lithium ion battery according to claim 1 is characterized in that, described electrode material comprises positive electrode or negative material, and described positive electrode adopts the lithium ion compound, and described lithium ion compound comprises LiMn
2O
4, Li
3V
2(PO4)
3, LiFeM
1PO
4, LiMnO
2, LiMnM
2O
2, LiFePO
4In one or more, M wherein
1Comprise Ni, Co, Mn, Mg, Ca, Cr, V, Sr, M
2Comprise Ni, Co, Mg, Ca, Cr, V, Sr, described negative material comprises material with carbon element, silicon materials, SiO
2, nitride, SnO
2, Sb
2O
3, Li
4Ti
5O
12In one or more, described material with carbon element comprises natural or artificial synthetic graphite, celion, carbonaceous mesophase spherules, hard carbon, carbon nano-tube, Graphene.
4. the electrode composite material of lithium ion battery according to claim 1 is characterized in that, described carbonization medium is space network, coats described collector and described electrode material.
5. the electrode composite material of lithium ion battery according to claim 1, it is characterized in that, described porous polymer glue comprises polyvinylidene fluoride, polytetrafluoroethylene, polyoxyethylene, polymethyl acrylate, have in the polymer of acrylate monomer one or more, the thickness of described porous polymer glue is 1 μ m-5 μ m, and viscosity is 0.1PaS-10PaS.
6. the electrode composite material of lithium ion battery according to claim 1 is characterized in that, described electrode composite material is flaky material, and thickness is 100 μ m-100cm.
7. the preparation method of the electrode composite material of lithium ion battery according to claim 1, it is characterized in that, comprise that step is: add adhesive and in solvent, make colloidal solution, add again electrode material and conductive agent, be stirred into the paste slurry, the slurry that obtains is filled in many seepage holes of collector, carry out the drying first time, be cast into certain thickness with Pressing device, in inert gas, calcine again, apply porous polymer glue at collection liquid surface after the cooling, carry out the drying second time, obtain the electrode composite material of lithium ion battery.
8. preparation method according to claim 7, it is characterized in that, described adhesive comprises one or more in polyethylene, polypropylene, polybutadiene, sodium carboxymethylcellulose, polyvinylidene fluoride, polytetrafluoroethylene, polyacrylonitrile, ethylene propylene diene rubber, synthetic rubber, the polyurethane, and described conductive agent comprises carbon black, acetylene black, carbon nano-tube, ultra-fine carbon dust or gas-phase growth of carbon fibre.
9. preparation method according to claim 7, it is characterized in that, dry and the described second time of the described first time, the temperature of drying was 90 ℃-110 ℃, the dry time is 4h-12h for the first time, the dry time is 1h-10h for the second time, and described calcination process is to carry out 2h-8h under 500 ℃-1200 ℃.
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| CN111276668A (en) * | 2018-12-05 | 2020-06-12 | 丰田自动车株式会社 | Electrode laminate for all-solid-state battery and method for producing same |
| CN112467113A (en) * | 2020-12-01 | 2021-03-09 | 南昌大学 | Preparation method of nitrogen-doped carbon-coated silicon dioxide nanotube composite material |
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| Publication number | Publication date |
|---|---|
| CN102916161B (en) | 2016-02-17 |
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