CN104134779A - High voltage lithium ion battery positive pole piece and preparation method thereof - Google Patents
High voltage lithium ion battery positive pole piece and preparation method thereof Download PDFInfo
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- CN104134779A CN104134779A CN201410118372.4A CN201410118372A CN104134779A CN 104134779 A CN104134779 A CN 104134779A CN 201410118372 A CN201410118372 A CN 201410118372A CN 104134779 A CN104134779 A CN 104134779A
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- pole piece
- lithium ion
- active material
- ion batteries
- additive
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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
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/624—Electric conductive fillers
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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
-
- 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
- H01M4/131—Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
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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
- H01M4/136—Electrodes based on inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy
-
- 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
- H01M4/1391—Processes of manufacture of electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
-
- 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
- H01M4/1397—Processes of manufacture of electrodes based on inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Materials Engineering (AREA)
- Manufacturing & Machinery (AREA)
- Inorganic Chemistry (AREA)
- Battery Electrode And Active Subsutance (AREA)
Abstract
Belonging to the technical field of lithium ion batteries, the invention discloses a high voltage lithium ion battery positive pole piece and a preparation method thereof. The high voltage lithium ion battery positive pole piece comprises a positive current collector and an active material layer coating the positive current collector. The active material layer includes an active material, a binder and a conductive agent. The positive pole piece contains an electropolymerization additive, which is an organic compound able to form a conductive polymer at 4.1-4.9V(vs.Li/Li<+>). The active material in the positive pole piece is a positive material with a discharge platform higher than 4.5V(vs.Li/Li<+>). Adding of the electropolymerization additive into the battery pole piece can effectively reduce the interfacial reaction of the high voltage active material and an electrolyte solution, and also has more significant advantages than adding the electropolymerization additive into the electrolyte solution, and diaphragm hole plugging caused by the polymer generated in the electropolymerization process of the elctropolymerization additive can be effectively reduced, thus further improving the battery performance significantly.
Description
?
Technical field
the invention belongs to technical field of lithium ion, be specifically related to a kind of high-voltage lithium ion batteries anode pole piece and preparation method thereof.
Background technology
The anode material for lithium-ion batteries using at present, as LiCoO
2, LiMn
2o
4and LiFePO
4operating voltage all lower than 4V, with LiNi
0.5mn
1.5o
4and LiCoPO
4the discharge voltage of the high-voltage anode material that is representative Deng material can be up to 5V left and right, these high voltage materials can improve output voltage and the power density of battery for lithium ion battery, further widen lithium ion battery at high-power electrical equipment, especially the scope of application on electric automobile, thus be subject to researcher's extensive concern in the industry.The liquid electrolyte of commercial lithium-ion batteries is mainly the conventional carbonate group electrolyte based on ethylene carbonate (EC) at present, but when system voltage is during higher than 4.5V, thereby can there is to decompose the decline that causes whole battery performance in conventional carbonate group electrolyte solvent, and this problem can substitute carbonates solvent completely in the face of there is no other novel dissolvent, thereby the test that causes current high voltage material is the electrolyte solvent system based on conventional still, as EC/EMC/DMC, EC/DEC, EC/DMC and EC/EMC etc.In order to solve high voltage material and the electrolyte matching problem in battery, many employing Al of bibliographical information
2o
3, ZrO
2, AlPO
4, ZnO, TiO
2, MgO, Bi
2o
3, BiOF, Li
3pO
4, the coating such as Lipon and LLTO comes LiNi
0.5mn
1.5o
4deng high-voltage anode material, be coated, from the surface of material particle, add coating, reduction particle contacts with electrolyte, reducing electrolyte oxidation decomposes, thereby improve the stability of mating between positive electrode and electrolyte, but cladding process is comparatively loaded down with trivial details, and coated inhomogeneous.
?
Summary of the invention
The object of the present invention is to provide a kind of high-voltage lithium ion batteries anode pole piece and preparation method thereof.
Object of the present invention can be achieved through the following technical solutions:
A kind of high-voltage lithium ion batteries anode pole piece, comprise plus plate current-collecting body and be coated in the active material layer on plus plate current-collecting body, described active material layer comprises active material, binding agent and conductive agent, it is characterized in that, contains electropolymerization additive in described anode pole piece; Described electropolymerization additive is to form at 4.1-4.9V (vs.Li/Li+) organic compound of conducting polymer; In described anode pole piece, active material is that discharge platform is higher than the positive electrode of 4.5V (vs.Li/Li+).
Nickel LiMn2O4, iron LiMn2O4, cobalt manganic acid lithium that described discharge platform is spinel structure higher than the positive electrode of 4.5V (vs. Li/Li+), one or more mixtures in the vanadic acid nickel lithium of the cobalt phosphate lithium of olivine structural, LiNiPO, fluorophosphoric acid cobalt lithium and inverse spinel structure.
The described organic compound that can form conducting polymer at 4.1-4.9V (vs. Li/Li+) be boiling point higher than the benzene-like compounds of 250 ℃.
Described boiling point is one or more mixtures in connection benzene and its derivative, adjacent diphenyl benzene and its derivative, diphenyl ether and derivative, bibenzyl and derivative thereof higher than the benzene-like compounds of 250 ℃.
The invention also discloses a kind of preparation method of high pressure anode slice of lithium ion battery, the method is specially: electropolymerization additive is dissolved in 100 parts of 1-METHYLPYRROLIDONE solvents, add 1-10 part binding agent, under vacuum condition, uniform stirring is made glue, then in glue, add 1-15 part conductive agent, vacuum stirring 1-4h, add again 75-98 part active material vacuum stirring 2-10h, with 1-METHYLPYRROLIDONE, regulating mixture solid content is 30-70%, mixture is evenly coated on collector aluminium foil by coating machine, drying, after roll-in, obtain high-voltage lithium ion batteries anode pole piece.
The mass ratio of described electropolymerization additive and active material is 0.001-5:100.
The mass ratio of described electropolymerization additive and active material is preferably 0.05-0.5:100.
Described conductive agent is one or more mixtures in graphite, acetylene black, carbon fiber, carbon nano-tube and Ketjen black.
Described binding agent is one or more mixtures in PVDF, PVDF-HFP, PEO, PMMA, PAN, PVA.
Beneficial effect of the present invention:
1, the present invention mixes electropolymerization additive in anode pole piece, utilize electropolymerization additive, in battery charging process, the principle of electrochemical polymerization can occur, the original position that realizes high-voltage positive electrode material is evenly coated, this polymer can intercept high-voltage anode active material and contact with the direct of electrolyte under the prerequisite that does not affect the de-embedding of lithium ion, reduces the high pressure oxidation interface side reaction of electrolyte.
2, the present invention adds electropolymerization additive in battery pole piece, can effectively reduce the interfacial reaction of high voltage active material and electrolyte, in electrolyte, adding electropolymerization additive more there is significant advantage simultaneously, can effectively reduce the polymer plugging barrier film hole that electropolymerization additive produces in electropolymerization process, further obviously improve battery performance.
Embodiment
Below in conjunction with specific embodiment, the present invention is described in further detail.
Embodiment 1:
8g biphenyl is joined in 1kg 1-METHYLPYRROLIDONE, under vacuum, mix, add again 80g binding agent PVDF(HSV900 type) make glue under vacuum, again in active material: conductive agent: the ratio of binding agent mass ratio=94:3.5:2.5, by 3 kg nickel LiMn2O4s and 96g acetylene black, the agent of 16g graphite joins in 1-METHYLPYRROLIDONE, vacuum is mixed 5h, with 1-METHYLPYRROLIDONE, regulating slurry solid content is again 6000cps left and right in 41%(viscosity), then this slurry be evenly coated on 20um aluminium foil on coating machine and be dried, according to experimental technique, dry pole piece obtains compacted density on roll squeezer after roll-in be 2.5g/cm
3nickel lithium manganate cathode pole piece.
Embodiment 2:
The adjacent diphenyl benzene of 4g is joined in 1kg 1-METHYLPYRROLIDONE, under vacuum, mix, add again 176g binding agent PVDF(HSV900 type) make glue under vacuum, again in mass ratio for active material: the ratio of conductive agent: binding agent=85:10:5 joins 3 kg nickel LiMn2O4s and 176g acetylene black and the agent of 176g graphite in 1-METHYLPYRROLIDONE, vacuum is mixed 10h, with 1-METHYLPYRROLIDONE, regulating slurry solid content is again 8000cps left and right in 37%(viscosity), then this slurry be evenly coated on 20um aluminium foil on coating machine and be dried, according to experimental technique, dry pole piece obtains compacted density on roll squeezer after roll-in be 2.3g/cm
3nickel lithium manganate cathode pole piece.
Embodiment 3:
16g bibenzyl is joined in 1kg 1-METHYLPYRROLIDONE, under vacuum, mix, add again 80g binding agent PVDF(HSV900 type) make glue under vacuum, be active material more in mass ratio: the ratio of conductive agent: binding agent=94:3.5:2.5 is by 3 kg nickel LiMn2O4s and 96g acetylene black, the agent of 16g graphite joins in 1-METHYLPYRROLIDONE, vacuum is mixed 5h, with 1-METHYLPYRROLIDONE, regulating slurry solid content is again 6000cps left and right in 42%(viscosity), then this slurry be evenly coated on 20um aluminium foil on coating machine and be dried, according to experimental technique, dry pole piece obtains compacted density on roll squeezer after roll-in be 2.5g/cm
3nickel lithium manganate cathode pole piece.
Embodiment 4:
The adjacent diphenyl benzene of 4g is joined in 1kg 1-METHYLPYRROLIDONE, under vacuum, mix, add again 100g binding agent PVDF(HSV900 type) make glue under vacuum, be active material more in mass ratio: the ratio of conductive agent: binding agent=85:10:5 is by 3 kg cobalt phosphate lithiums and 176g acetylene black, the agent of 176g graphite is by joining in NMP, vacuum is mixed 10h, with 1-METHYLPYRROLIDONE, regulating slurry solid content is again 8000cps left and right in 41%(viscosity), then this slurry be evenly coated on 20um aluminium foil on coating machine and be dried, according to experimental technique, dry pole piece obtains the cobalt phosphate lithium anode pole piece that compacted density is 2.1g/cm3 on roll squeezer after roll-in.
Embodiment 5:
7g biphenyl is joined in 1kg 1-METHYLPYRROLIDONE, under vacuum, mix, add again under 80g binding agent PVDF-HFP vacuum and make glue, be active material more in mass ratio: the ratio of conductive agent: binding agent=90:5:5 is by 3 kg LiNiPOs and 100g acetylene black, the agent of 67g carbon nanotube conducting joins in 1-METHYLPYRROLIDONE, vacuum is mixed 7h, with 1-METHYLPYRROLIDONE, regulating slurry solid content is again 6000cps left and right in 39%(viscosity), then this slurry be evenly coated on 20um aluminium foil on coating machine and be dried, according to experimental technique, dry pole piece obtains the LiNiPO anode pole piece that compacted density is 2.3g/cm3 on roll squeezer after roll-in.
Embodiment 6
By positive electrode, be spinel structure nickel LiMn2O4, iron LiMn2O4, cobalt manganic acid lithium, one or more mixtures in the vanadic acid nickel lithium of the cobalt phosphate lithium of olivine structural, LiNiPO, fluorophosphoric acid cobalt lithium and inverse spinel structure; By in electropolymerization additive biphenyl and derivative, adjacent diphenyl benzene and its derivative, diphenyl ether and derivative, bibenzyl and derivative thereof or several mixtures; Conductive agent is one or more mixtures in graphite, acetylene black, carbon fiber, carbon nano-tube or Ketjen black; Binding agent is at least one or several mixture in PVDF, PVDF-HFP, PEO, PMMA, PAN, PVA, according to above-described embodiment 1,2,3,4,5 steps, carry out, the anode pole piece of positive electrode under can obtaining, no further details to be given herein, in every case the equalization of doing according to the claims in the present invention scope changes and modifies, and all should belong to the covering scope of the claims in the present invention.
Comparative example:
By 80g binding agent PVDF(HSV900 type) join in 1kg 1-METHYLPYRROLIDONE, under vacuum, mix, make glue, again in mass ratio for the ratio of 94:3:2.5:0.5 joins 3kg nickel LiMn2O4 and 96g acetylene black and the agent of 16g carbon nanotube conducting in 1-METHYLPYRROLIDONE, vacuum is mixed 5h, with 1-METHYLPYRROLIDONE, regulating slurry solid content is again 6300cps left and right in 41%(viscosity), then this slurry be evenly coated on 20um aluminium foil on coating machine and be dried, according to experimental technique, dry pole piece obtains compacted density on roll squeezer after roll-in be 2.5g/cm
3contrast experiment with nickel lithium manganate cathode pole piece.
18650 batteries are made and are characterized:
Graphite, SP, SBR and CMC are joined in distilled water in certain sequence for the ratio of 93.2:2.5:2.5:1.8 in mass ratio, vacuum is mixed 5h, water regulates slurry viscosity to 4000cps left and right again, then this slurry be evenly coated on 12um Copper Foil on coating machine and be dried, according to experimental technique, dry pole piece obtains compacted density on roll squeezer after roll-in be 1.45g/cm
3graphite cathode pole piece.Control N/P=1.2, by embodiment 1 and comparative example's LiNi
0.5mn
1.5o
4anode pole piece and graphite cathode sheet are assembled into 18650 cylindrical batteries, barrier film adopts U.S. Entek25um polyalkene diaphragm, characterizing battery performance on BTS-2000 battery charging and discharging tester, discharging and recharging interval is 3.5V-4.8V, charge-discharge magnification is 0.33C, and test is respectively 1M LiPF with electrolyte
6eC/DEC/DMC(1:1:1) common electrolyte.Test result shows, 1860 batteries of assembling with the positive plate of embodiment 1, and after 100 circulations, capability retention is 85%; And take the prepared electrode plates of comparative example, to be assembled into capability retention after 100 times of 18650 batteries circulations be 67%.
By the above results, can be found out, the high-voltage lithium ion batteries pole piece that adopts the present invention to prepare, can effectively improve the cycle life of battery under high voltage condition, significant to the development of following lithium ion battery.
The foregoing is only preferred embodiment of the present invention, all equalizations of doing according to the claims in the present invention scope change and modify, and all should belong to the covering scope of the claims in the present invention.
Claims (9)
1. a high-voltage lithium ion batteries anode pole piece, comprise collector aluminium foil, it is characterized in that, on described collector aluminium foil, be coated with electropolymerization additive and active material, described electropolymerization additive is in 4.1-4.9V (vs.Li/Li+), to form the organic compound of conducting polymer, and described active material is that discharge platform is higher than the positive electrode of 4.5V (vs.Li/Li+).
2. high-voltage lithium ion batteries anode pole piece according to claim 1, it is characterized in that, nickel LiMn2O4, iron LiMn2O4, cobalt manganic acid lithium that described discharge platform is spinel structure higher than the positive electrode of 4.5V (vs. Li/Li+), one or more mixtures in the vanadic acid nickel lithium of the cobalt phosphate lithium of olivine structural, LiNiPO, fluorophosphoric acid cobalt lithium and inverse spinel structure.
3. high-voltage lithium ion batteries anode pole piece according to claim 1, is characterized in that, the described organic compound that can form conducting polymer in 4.1-4.9V (vs. Li/Li+) is boiling point higher than the benzene-like compounds of 250 ℃.
4. high-voltage lithium ion batteries anode pole piece according to claim 3, it is characterized in that, described boiling point is one or more mixtures in connection benzene and its derivative, adjacent diphenyl benzene and its derivative, diphenyl ether and derivative, bibenzyl and derivative thereof higher than the benzene-like compounds of 250 ℃.
5. the preparation method of a high-voltage lithium ion batteries anode pole piece as described in claim 1 or 2 or 3, it is characterized in that, the method is specially: electropolymerization additive is dissolved in 100 parts of 1-METHYLPYRROLIDONE solvents, add 1-10 part binding agent, under vacuum condition, uniform stirring is made glue, then in glue, add 1-15 part conductive agent, vacuum stirring 1-4h, add again 75-98 part active material vacuum stirring 2-10h, with 1-METHYLPYRROLIDONE, regulating mixture solid content is 30-70%, mixture is evenly coated on collector aluminium foil by coating machine, drying, after roll-in, obtain high-voltage lithium ion batteries anode pole piece.
?
6. method according to claim 5, is characterized in that, the mass ratio of described electropolymerization additive and active material is 0.001-5:100.
7. method according to claim 6, is characterized in that, the mass ratio of described electropolymerization additive and active material is preferably 0.05-0.5:100.
8. method according to claim 5, is characterized in that, described conductive agent is one or more mixtures in graphite, acetylene black, carbon fiber, carbon nano-tube or Ketjen black.
9. method according to claim 5, is characterized in that, described binding agent is at least one or several mixture in PVDF, PVDF-HFP, PEO, PMMA, PAN, PVA.
?
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201410118372.4A CN104134779A (en) | 2014-03-27 | 2014-03-27 | High voltage lithium ion battery positive pole piece and preparation method thereof |
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|---|---|---|---|
| CN201410118372.4A CN104134779A (en) | 2014-03-27 | 2014-03-27 | High voltage lithium ion battery positive pole piece and preparation method thereof |
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN108075114A (en) * | 2016-11-18 | 2018-05-25 | 株式会社半导体能源研究所 | Positive active material, the manufacturing method of positive active material and secondary cell |
| WO2018113438A1 (en) * | 2016-12-19 | 2018-06-28 | 苏州格瑞动力电源科技有限公司 | Preparation method for electrode slice of lithium ion battery |
| CN109994707A (en) * | 2017-12-29 | 2019-07-09 | 宁德时代新能源科技股份有限公司 | Positive plate, preparation method thereof and battery |
| CN109994708A (en) * | 2017-12-29 | 2019-07-09 | 宁德时代新能源科技股份有限公司 | Negative pole piece, preparation method thereof and secondary battery |
| CN111697186A (en) * | 2019-03-15 | 2020-09-22 | 深圳格林德能源集团有限公司 | High-energy-density lithium ion battery |
| CN112103514A (en) * | 2020-08-28 | 2020-12-18 | 深圳供电局有限公司 | Current collector, battery electrode, preparation method and battery |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN108075114A (en) * | 2016-11-18 | 2018-05-25 | 株式会社半导体能源研究所 | Positive active material, the manufacturing method of positive active material and secondary cell |
| WO2018113438A1 (en) * | 2016-12-19 | 2018-06-28 | 苏州格瑞动力电源科技有限公司 | Preparation method for electrode slice of lithium ion battery |
| CN109994707A (en) * | 2017-12-29 | 2019-07-09 | 宁德时代新能源科技股份有限公司 | Positive plate, preparation method thereof and battery |
| CN109994708A (en) * | 2017-12-29 | 2019-07-09 | 宁德时代新能源科技股份有限公司 | Negative pole piece, preparation method thereof and secondary battery |
| CN109994708B (en) * | 2017-12-29 | 2021-07-13 | 宁德时代新能源科技股份有限公司 | Negative pole piece, preparation method thereof and secondary battery |
| CN109994707B (en) * | 2017-12-29 | 2021-09-21 | 宁德时代新能源科技股份有限公司 | Positive plate, preparation method thereof and battery |
| CN111697186A (en) * | 2019-03-15 | 2020-09-22 | 深圳格林德能源集团有限公司 | High-energy-density lithium ion battery |
| CN112103514A (en) * | 2020-08-28 | 2020-12-18 | 深圳供电局有限公司 | Current collector, battery electrode, preparation method and battery |
| CN112103514B (en) * | 2020-08-28 | 2022-05-17 | 深圳供电局有限公司 | Current collector, battery electrode, preparation method and battery |
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Application publication date: 20141105 |