CN104319379B - A kind of lithium ion battery negative material preparation method and application - Google Patents
A kind of lithium ion battery negative material preparation method and application Download PDFInfo
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- CN104319379B CN104319379B CN201410566562.2A CN201410566562A CN104319379B CN 104319379 B CN104319379 B CN 104319379B CN 201410566562 A CN201410566562 A CN 201410566562A CN 104319379 B CN104319379 B CN 104319379B
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- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims abstract description 31
- 229910001416 lithium ion Inorganic materials 0.000 title claims abstract description 31
- 239000000463 material Substances 0.000 title claims abstract description 26
- 238000002360 preparation method Methods 0.000 title claims abstract description 16
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 42
- 229910052799 carbon Inorganic materials 0.000 claims abstract description 40
- KAESVJOAVNADME-UHFFFAOYSA-N Pyrrole Chemical compound C=1C=CNC=1 KAESVJOAVNADME-UHFFFAOYSA-N 0.000 claims abstract description 30
- 150000001875 compounds Chemical class 0.000 claims abstract description 26
- 239000000178 monomer Substances 0.000 claims abstract description 15
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims abstract description 7
- 229910052744 lithium Inorganic materials 0.000 claims abstract description 7
- 238000000034 method Methods 0.000 claims abstract description 7
- 238000005406 washing Methods 0.000 claims abstract description 7
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 52
- 239000004408 titanium dioxide Substances 0.000 claims description 26
- 229920000128 polypyrrole Polymers 0.000 claims description 15
- 238000006243 chemical reaction Methods 0.000 claims description 13
- 239000007864 aqueous solution Substances 0.000 claims description 9
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 7
- 239000003792 electrolyte Substances 0.000 claims description 6
- 230000035484 reaction time Effects 0.000 claims description 6
- 238000005119 centrifugation Methods 0.000 claims description 5
- 230000004044 response Effects 0.000 claims description 5
- 239000007787 solid Substances 0.000 claims description 5
- QGHDLJAZIIFENW-UHFFFAOYSA-N 4-[1,1,1,3,3,3-hexafluoro-2-(4-hydroxy-3-prop-2-enylphenyl)propan-2-yl]-2-prop-2-enylphenol Chemical group C1=C(CC=C)C(O)=CC=C1C(C(F)(F)F)(C(F)(F)F)C1=CC=C(O)C(CC=C)=C1 QGHDLJAZIIFENW-UHFFFAOYSA-N 0.000 claims description 4
- WQZGKKKJIJFFOK-GASJEMHNSA-N Glucose Natural products OC[C@H]1OC(O)[C@H](O)[C@@H](O)[C@@H]1O WQZGKKKJIJFFOK-GASJEMHNSA-N 0.000 claims description 4
- 229910019142 PO4 Inorganic materials 0.000 claims description 4
- WQZGKKKJIJFFOK-VFUOTHLCSA-N beta-D-glucose Chemical compound OC[C@H]1O[C@@H](O)[C@H](O)[C@@H](O)[C@@H]1O WQZGKKKJIJFFOK-VFUOTHLCSA-N 0.000 claims description 4
- 239000012153 distilled water Substances 0.000 claims description 4
- 239000008103 glucose Substances 0.000 claims description 4
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 claims description 4
- 239000010452 phosphate Substances 0.000 claims description 4
- OTYBMLCTZGSZBG-UHFFFAOYSA-L potassium sulfate Chemical compound [K+].[K+].[O-]S([O-])(=O)=O OTYBMLCTZGSZBG-UHFFFAOYSA-L 0.000 claims description 4
- 229910052939 potassium sulfate Inorganic materials 0.000 claims description 4
- 235000011151 potassium sulphates Nutrition 0.000 claims description 4
- 238000002242 deionisation method Methods 0.000 claims description 2
- 238000004519 manufacturing process Methods 0.000 abstract description 6
- 239000010406 cathode material Substances 0.000 abstract description 4
- 229910044991 metal oxide Inorganic materials 0.000 abstract description 3
- 150000004706 metal oxides Chemical class 0.000 abstract description 3
- 238000007086 side reaction Methods 0.000 abstract description 3
- 238000001035 drying Methods 0.000 abstract description 2
- 238000005265 energy consumption Methods 0.000 abstract description 2
- 230000001988 toxicity Effects 0.000 abstract description 2
- 231100000419 toxicity Toxicity 0.000 abstract description 2
- 150000002500 ions Chemical class 0.000 abstract 1
- 229910000314 transition metal oxide Inorganic materials 0.000 description 7
- 239000000243 solution Substances 0.000 description 5
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 description 4
- 229910052804 chromium Inorganic materials 0.000 description 4
- 239000011651 chromium Substances 0.000 description 4
- 239000008367 deionised water Substances 0.000 description 3
- 229910021641 deionized water Inorganic materials 0.000 description 3
- HMDDXIMCDZRSNE-UHFFFAOYSA-N [C].[Si] Chemical compound [C].[Si] HMDDXIMCDZRSNE-UHFFFAOYSA-N 0.000 description 2
- 230000004888 barrier function Effects 0.000 description 2
- 230000004087 circulation Effects 0.000 description 2
- 239000002131 composite material Substances 0.000 description 2
- QSNQXZYQEIKDPU-UHFFFAOYSA-N [Li].[Fe] Chemical compound [Li].[Fe] QSNQXZYQEIKDPU-UHFFFAOYSA-N 0.000 description 1
- 239000000956 alloy Substances 0.000 description 1
- 239000006229 carbon black Substances 0.000 description 1
- 230000006835 compression Effects 0.000 description 1
- 238000007906 compression Methods 0.000 description 1
- 230000007812 deficiency Effects 0.000 description 1
- 210000001787 dendrite Anatomy 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000004146 energy storage Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 239000000835 fiber Substances 0.000 description 1
- 239000010439 graphite Substances 0.000 description 1
- 229910002804 graphite Inorganic materials 0.000 description 1
- 230000014759 maintenance of location Effects 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 229920000915 polyvinyl chloride Polymers 0.000 description 1
- 239000004800 polyvinyl chloride Substances 0.000 description 1
- 230000001376 precipitating effect Effects 0.000 description 1
- 230000008569 process Effects 0.000 description 1
- 239000002210 silicon-based material Substances 0.000 description 1
- 239000011366 tin-based material Substances 0.000 description 1
Classifications
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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
-
- 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
- H01M4/139—Processes of manufacture
-
- 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
- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
- H01M4/483—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides for non-aqueous cells
-
- 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)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Manufacturing & Machinery (AREA)
- Composite Materials (AREA)
- Inorganic Chemistry (AREA)
- Battery Electrode And Active Subsutance (AREA)
Abstract
The present invention relates to a kind of lithium ion battery negative material preparation method and application.This compound is by after pyrrole monomer and carbon doping reactive metal oxide, by being simply separated, washing and drying can obtain, the compound obtained has large, the high cyclical stability of specific capacity, toxicity is little, energy consumption is low, is a kind of ion cathode material lithium of good performance.The preparation method of this compound simultaneously, easy and simple to handle, environmentally safe, does not have side reaction, with low cost, is a kind of practicable method, is convenient to the use of this compound.The advantage the invention still further relates to a kind of preparation method of carbon doping metal oxide, the method has that production cost is low, feasibility is large, being easy to realize industrial mass manufacture.
Description
Technical field
The invention belongs to field of electrochemical power source, be specifically related to a kind of cathode material of lithium ion battery preparation method and application.
Background technology
Lithium ion battery has that lot of advantages is as high in voltage, the volume little life-span is long etc., and it has progressively entered into new-energy automobile field and energy-storage battery field, becomes the emphasis of electrochemical field research.
Lithium ion battery mainly comprises four parts usually: positive pole, negative pole, electrolyte and barrier film, electrolyte primary attachment is in barrier film, it is the carrier of lithium ion movement between positive/negative plate, the negative material that current lithium ion battery uses is mainly carbon negative pole material, as electrographite, native graphite etc., but because material with carbon element exists the shortcoming such as larger energy loss and high-rate charge-discharge capability difference, the easy precipitating metal lithium of carbon electrodes simultaneously, form dendrite and cause short circuit, therefore, the goal in research of people be find more reliable, more efficient novel lithium battery cathode material.Report a large amount of non-carbon negative material in recent years as lithium iron composite material, tin-based material, silica-base material and other novel alloy material.As Chinese patent CN103367727A reports the lithium ion battery of silicon-carbon cathode material, the specific capacity of prepared carbon silicon materials is greater than 450mAh/g, and efficiency is greater than 85% first, circulates 60 capability retentions more than 97%.Chinese patent CN103456934A discloses a kind of carbon doping titanium dioxide/carbon composite fibre for lithium ion battery negative material, and the battery of gained first discharge capacity is 353 ~ 364mAh/g, and the charging capacity after 100 circulations is 268mAh/g.
Summary of the invention
Just in order to solve the deficiencies in the prior art, the invention provides and a kind ofly there is height ratio capacity and repeatedly still have lithium ion battery negative material compared with charge capacity after circulation.A kind of method that another object of the present invention provides easy and simple to handle, environmentally safe, there is not side reaction, prepares lithium ion battery negative material carbon doping transition metal oxide and polypyrrole compound inexpensively.The preparation method preparing carbon doping titanium dioxide that 3rd object of the present invention is to provide that a kind of production cost is low, feasibility is large, be easy to realize industrial mass manufacture.
For realizing above object, the invention provides following technical scheme:
A kind of lithium ion battery negative material preparation method, is characterized in that,
(1) compound concentration is the pyrrole monomer aqueous solution of 0.01 ~ 0.5M, ultrasonic 0.5 ~ 1 hour;
(2), after adding carbon doping transition metal oxide in the chromium solution of step (1) gained, after ultrasonic 10 ~ 20 minutes, react in microwave;
(3) after question response terminates, obtain solid by centrifugation, then after deionization washing, place in baking oven, oven temperature is 100 ~ 200 DEG C, obtains the compound of carbon doping metal oxide and polypyrrole after dry 1 ~ 2 hour.
Described carbon doping transition metal oxide is preferably carbon doping titanium dioxide, and the mass ratio of described pyrrole monomer and carbon doping titanium dioxide is 1:5 ~ 5:1.
Wherein, described carbon doping titanium dioxide obtains by the following method: take TiCl successively for 1:0.2 ~ 0.5:0.1 ~ 0.2 in mass ratio
3, glucose and potassium sulfate join in the distilled water of 20 ~ 30 parts of weight ratios, after being fully uniformly mixed, mixed liquor is joined in hydrothermal reactor, isothermal reaction at 120 ~ 180 DEG C, the reaction time is 5 ~ 15 hours, and obtained carbon doping titanium dioxide is dried in the washing of gained material.
Wherein, in step (1), compound concentration is the pyrrole monomer aqueous solution of 0.05 ~ 0.2M, and the power reacted in step (2) microwave is 120 ~ 160KW, and reaction temperature is 80 ~ 120 DEG C, 5 ~ 15 minutes reaction time.In step (3), oven temperature is 120 ~ 180 DEG C.
The compound of the carbon doping transition metal oxide that the preparation method of lithium ion battery negative material as above prepares and polypyrrole.
As above a kind of application of lithium ion battery negative material, it is characterized in that, get the compression of the compound of carbon doping transition metal oxide and polypyrrole, carbon black and polyvinyl chloride and make work electrode, lithium hexafluoro phosphate is as electrolyte, test the charge-discharge performance of this lithium ion battery, first charge-discharge capacity is 558 ~ 574mAh/g, and circulate 200 not decay, and the charging capacity after 400 times that circulates is 446 ~ 467mAh/g.
Technique effect: 1, the preparation method of negative material carbon doping titanium dioxide of the present invention and polypyrrole compound is simple, easy to operate, environmentally safe, does not have side reaction, with low cost.2, carbon doping titanium dioxide of the present invention and polypyrrole compound are applied to lithium ion battery, and large, the high cyclical stability of lithium ion battery specific capacity of gained, toxicity is little, energy consumption is low, good stability.3, the preparation method preparing carbon doping titanium dioxide the invention provides that a kind of production cost is low, feasibility is large, being easy to realize industrial mass manufacture.
Accompanying drawing explanation
Fig. 1 is a process chart of the present invention.
Embodiment
Embodiment 1
TiCl is taken successively in mass ratio for 1:0.3:0.1
3, glucose and potassium sulfate join in the distilled water of 20 parts of mass ratioes, after being fully uniformly mixed, mixed liquor is joined in hydrothermal reactor, isothermal reaction at 120 DEG C, the reaction time is about 10 hours, and obtained carbon doping titanium dioxide is dried in the washing of gained material.
Embodiment 2
TiCl is taken successively in mass ratio for 1:0.2:0.2
3, glucose and potassium sulfate join in the distilled water of 25 parts of mass ratioes, after being fully uniformly mixed, mixed liquor is joined in hydrothermal reactor, isothermal reaction at 160 DEG C, the reaction time is about 6 hours, and obtained carbon doping titanium dioxide is dried in the washing of gained material.
Embodiment 3
(1) take 1g pyrrole monomer, compound concentration is the pyrrole monomer aqueous solution of 0.1M, ultrasonic 30 minutes;
(2), add the obtained carbon doping titanium dioxide of 1.5g embodiment 1 in the chromium solution of step (1) gained after, after ultrasonic 10 minutes, reaction temperature is 120 DEG C, and reaction power is 120KW;
(3) after question response terminates, obtain solid by centrifugation, then after deionized water washs 3 times, place in baking oven, oven temperature is 120 DEG C, obtains the compound of carbon doping titanium dioxide and polypyrrole after after dry 2 hours.
Using the carbon doping transition metal oxide of gained and the compound of the polypyrrole work electrode as lithium ion battery, lithium hexafluoro phosphate is as electrolyte, test the charge-discharge performance of this lithium ion battery, with the current density discharge and recharge of 50mA/g, first charge-discharge capacity is 558mAh/g, circulate 200 not decay, and the charging capacity after 400 times that circulates is 446mAh/g.
Embodiment 4
(1) take 2g pyrrole monomer, compound concentration is the pyrrole monomer aqueous solution of 0.05M, ultrasonic 30 minutes;
(2), add the obtained carbon doping titanium dioxide 1.6g of 1g embodiment 2 in the chromium solution of step (1) gained after, after ultrasonic 10 minutes, react 5 minutes in microwave, reaction temperature is 100 DEG C, and reaction power is 160KW;
(3) after question response terminates, obtain solid by centrifugation, then after deionized water washs 3 times, place in baking oven, oven temperature is 150 DEG C, obtains the compound of carbon doping titanium dioxide and polypyrrole after after dry 1 hour.
Using the carbon doping transition metal oxide of gained and the compound of the polypyrrole work electrode as lithium ion battery, lithium hexafluoro phosphate is as electrolyte, test the charge-discharge performance of this lithium ion battery, with the current density discharge and recharge of 50mA/g, first charge-discharge capacity is 574mAh/g, circulate 200 not decay, and the charging capacity after 400 times that circulates is 467mAh/g.
Embodiment 5
(1) take 1g pyrrole monomer, compound concentration is the pyrrole monomer aqueous solution of 0.01M, ultrasonic 35 minutes;
(2), add the obtained carbon doping titanium dioxide 1.6g of 2g embodiment 1 in the chromium solution of step (1) gained after, after ultrasonic 15 minutes, react 5 minutes in microwave, reaction temperature is 100 DEG C, and reaction power is 160KW;
(3) after question response terminates, obtain solid by centrifugation, then after deionized water washs 3 times, place in baking oven, oven temperature is 140 DEG C, obtains the compound of carbon doping titanium dioxide and polypyrrole after dry 1.5 hours.
In a word, above-described embodiment is only better embodiment of the present invention, in enforcement of the present invention, 1. the concentration of the pyrrole monomer aqueous solution of first step is an optional concentration value between 0.01M, 0.03M, 0.05M, 0.1M, 0.2M, 0.3M, 0.4M, 0.5M; 2. in the second step, after adding carbon doping titanium dioxide, an optional time value between ultrasonic 10 minutes, 12 minutes, 15 minutes, 18 minutes, 20 minutes, 25 minutes, and in microwave, react a selection time value between 3 minutes, 5 minutes, 8 minutes, 10 minutes, 15 minutes, 18 minutes, 20 minutes, reaction temperature is select a temperature arbitrarily between 100 DEG C, 120 DEG C, 140 DEG C, 150 DEG C, 160 DEG C, 180 DEG C, 200 DEG C.In third step, oven temperature is select a temperature value between 100 DEG C, 120 DEG C, 140 DEG C, 150 DEG C, 160 DEG C, 180 DEG C, within dry 1 hour, 1.2 hours, 1.5 hours, 1.8 hours, 2 hours, selects a drying time values.The combination in any of the parameter in above-mentioned 1,2,3 three condition, all belongs in interest field of the present invention.
Above-described embodiment not imposes any restrictions technical scope of the present invention.The technical staff of the industry, under the inspiration of the technical program, some distortion and amendment can be made, every above embodiment is done according to technical spirit of the present invention any amendment, equivalent variations and modification, all still belong in the scope of technical solution of the present invention.
Claims (5)
1. a lithium ion battery negative material preparation method, it is characterized in that described lithium ion battery negative material is the compound of carbon doping titanium dioxide and polypyrrole, and described preparation method comprises the following steps:
(1) compound concentration is the pyrrole monomer aqueous solution of 0.01 ~ 0.5M, ultrasonic 0.5 ~ 1 hour;
(2) in the pyrrole monomer aqueous solution of step (1) gained, add carbon doping titanium dioxide, after ultrasonic 10 ~ 20 minutes, react in microwave;
(3) after question response terminates, obtain solid by centrifugation, then after deionization washing, place in baking oven, oven temperature is 100 ~ 200 DEG C, obtains the compound of carbon doping titanium dioxide and polypyrrole after dry 1-2 hour; Wherein, described carbon doping titanium dioxide obtains by the following method: take TiCl successively for 1:0.2 ~ 0.5:0.1 ~ 0.2 in mass ratio
3, glucose and potassium sulfate join in appropriate distilled water, after being fully uniformly mixed, mixed liquor is joined in hydrothermal reactor, isothermal reaction at 120 ~ 180 DEG C, the reaction time is 5 ~ 15 hours, the washing of gained material is dried i.e. obtained described carbon doping titanium dioxide.
2. a kind of lithium ion battery negative material preparation method according to claim 1, it is characterized in that, the mass ratio of described pyrrole monomer and carbon doping titanium dioxide is 1:5 ~ 5:1, the power reacted in step (2) microwave is 120 ~ 160KW, reaction temperature is 80 ~ 120 DEG C, 5 ~ 15 minutes reaction time.
3. a kind of lithium ion battery negative material preparation method according to claim 1 and 2, it is characterized in that, in step (1), compound concentration is the pyrrole monomer aqueous solution of 0.05 ~ 0.2M, and in step (3), oven temperature is 120 ~ 180 DEG C.
4., according to the lithium ion battery negative material that the arbitrary described preparation method of claim 1-3 prepares, described lithium ion battery negative material is the compound of carbon doping titanium dioxide and polypyrrole.
5. the application of lithium ion battery negative material according to claim 4, it is characterized in that: the work electrode of compound as lithium ion battery getting carbon doping titanium dioxide and polypyrrole, lithium hexafluoro phosphate is as electrolyte, test the charge-discharge performance of this lithium ion battery, with the current density discharge and recharge of 50mA/g, first charge-discharge capacity is 558 ~ 574mAh/g, and circulate 200 not decay, and the charging capacity after 400 times that circulates is 446 ~ 467mAh/g.
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Effective date of registration: 20150916 Address after: Longhua District, Dalang street, Tong Sheng community Huarong Road dragon 518000 Guangdong province rich city of Shenzhen industrial zone 3 building 1-3 layer Applicant after: GUANGDONG TIANJIN NEW ENERGY TECHNOLOGY Ltd. Address before: 518033 Futian District, Guangdong, Shennan Road, No., international culture building, room 1018, room 3039 Applicant before: Chen Buxiao |
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