WO2014168327A1 - 리튬 이차전지용 음극, 그 제조방법 및 이를 포함하는 리튬 이차전지 - Google Patents
리튬 이차전지용 음극, 그 제조방법 및 이를 포함하는 리튬 이차전지 Download PDFInfo
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- WO2014168327A1 WO2014168327A1 PCT/KR2014/001054 KR2014001054W WO2014168327A1 WO 2014168327 A1 WO2014168327 A1 WO 2014168327A1 KR 2014001054 W KR2014001054 W KR 2014001054W WO 2014168327 A1 WO2014168327 A1 WO 2014168327A1
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- negative electrode
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- carbon
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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
- H01M4/137—Electrodes based on electro-active polymers
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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
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/04—Processes of manufacture in general
- H01M4/0402—Methods of deposition of the material
- H01M4/0404—Methods of deposition of the material by coating on electrode collectors
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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
- H01M4/133—Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/139—Processes of manufacture
- H01M4/1393—Processes of manufacture of electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
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- H—ELECTRICITY
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- 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
- H01M4/1399—Processes of manufacture of electrodes based on electro-active polymers
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
- H01M4/583—Carbonaceous material, e.g. graphite-intercalation compounds or CFx
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
- H01M4/583—Carbonaceous material, e.g. graphite-intercalation compounds or CFx
- H01M4/587—Carbonaceous material, e.g. graphite-intercalation compounds or CFx for inserting or intercalating light metals
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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
- H01M4/621—Binders
- H01M4/622—Binders being polymers
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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
- H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
- H01M2004/027—Negative electrodes
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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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- 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
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
Definitions
- the present invention relates to a negative electrode for a lithium secondary battery, a method for manufacturing the same, and a lithium secondary battery including the same, and more particularly, to a negative electrode for a lithium secondary battery including a conductive polymer, a method for manufacturing the same, and a lithium secondary battery including the same.
- a lithium secondary battery includes a negative electrode made of a carbon material or a lithium metal alloy, a positive electrode made of a lithium metal oxide, and an electrolyte in which lithium salt is dissolved in an organic solvent.
- a negative electrode active material constituting a negative electrode of a lithium secondary battery Initially lithium metal was used.
- lithium has a problem of low reversibility and safety, and carbon materials are mainly used as negative electrode active materials of lithium secondary batteries. Carbon materials have a smaller capacity than lithium metal, but have a small volume change, excellent reversibility, and an advantageous price.
- Such a carbon-based negative electrode active material has a limited conductivity, and when manufacturing the electrode, there is a disadvantage that increases the resistance of the electrode by forming an empty space at the boundary between the active material.
- Korean Patent Publication No. 2012-0129983 discloses a cathode material for improving conductivity using carbon black, but the manufacturing method is complicated. And there is a problem that the conductivity is also not enough.
- the present invention is to solve the problems of the prior art as described above,
- the purpose of the present invention is to supplement the shortcomings of the deterioration of the conductivity, which is a disadvantage of the carbon-based negative active material, and to provide a negative electrode for a lithium secondary battery that can easily manufacture the negative electrode.
- It includes a carbon-based negative electrode active material, a binder and a conductive polymer, the conductive polymer provides a negative electrode for a lithium secondary battery, characterized in that it has a fiber form.
- the present invention comprises the steps of preparing a slurry by dispersing the carbon-based negative electrode active material and the conductive polymer in a solution in which the binder is dissolved; (B) applying the slurry on the surface of the current collector on which the negative electrode active material layer is formed; And (C) drying the current collector applied in the step (B), wherein the conductive polymer has a fiber shape.
- the negative electrode for a lithium secondary battery according to the present invention by applying PEDOT / PSS as the conductive polymer, there is an advantage that it is possible to prevent a drop in conductivity, which is a disadvantage of the carbon-based negative electrode active material, and to easily control the production of the negative electrode.
- FIG. 1 is a view showing a schematic diagram of the manufacturing method of the present invention.
- Example 2 is a graph showing the life and efficiency characteristics of the battery prepared in Example 1 and Comparative Example 1 according to the present invention.
- Example 3 is a graph of the resistance characteristics of the battery prepared in Example 1 and Comparative Example 1 according to the present invention.
- the negative electrode for a lithium secondary battery according to the present invention includes a carbon-based negative electrode active material, a binder, and a conductive polymer, and the conductive polymer has a fiber shape.
- a carbon-based negative electrode active material conventionally used may be used.
- a carbonaceous material may be used as the carbon-based negative electrode active material, and as the carbonaceous material, both low crystalline carbon and high crystalline carbon may be used.
- the low crystalline carbon soft carbon and hard carbon are representative, and the high crystalline carbon is natural graphite, Kish graphite, pyrolytic carbon, liquid crystal pitch-based carbon.
- High-temperature calcined carbon such as fibers (mesophase pitch based carbon fiber), meso-carbon microbeads, liquid crystal pitch (Mesophase pitches) and petroleum or coal tar pitch derived cokes.
- the content range of the carbon-based negative electrode active material is not particularly limited as long as it is generally used, it may be included in an amount of 20 to 95% by weight relative to the total weight of the negative electrode.
- the content ratio of the carbon-based negative electrode active material satisfies the above range, the conductivity of the battery is excellent.
- Binders usable in the present invention include styrene-butadiene rubber (SBR), nitrile-butadiene rubber, methyl (meth) acrylate-butadiene rubber, chloroprene rubber, carboxy modified styrene-butadiene rubber, carboxy methylcellulose (CMC) and modified polyorgano Any one of the siloxane-based polymers or a mixture of two or more thereof may be used, preferably styrene-butadiene rubber.
- SBR styrene-butadiene rubber
- CMC carboxy methylcellulose
- the content range of the binder is not particularly limited as long as it is generally used, but the binder is included in the remaining amount such that the total weight of the entire negative electrode is 100% by weight, and may be adjusted according to the content of other components. Can be.
- PEDOT / PSS poly-3,4-ethylenedioxythiophene / polystyrenesulfonate
- the PEDOT / PSS poly-3,4-ethylenedioxythiophene / polystyrenesulfonate
- the conductive polymer may be included in an amount of 0.1 to 3% by weight, preferably 0.5 to 2% by weight, and more preferably 0.8 to 1.5% by weight, based on the solid content of the negative electrode.
- the content ratio of the conductive polymer satisfies the above range, there is an advantage in that the conductivity is prevented from dropping and the preparation of the negative electrode can be easily controlled.
- the manufacturing method of the negative electrode according to the present invention is not particularly limited, and may be prepared by applying and drying a conventional method known in the art, that is, an electrode slurry including a negative electrode active material, a binder, and a conductive polymer on a current collector. At this time, a dispersing agent or surfactant may be used as needed.
- a lithium secondary battery according to the present invention includes a negative electrode including a carbon-based negative electrode active material for non-carbon lithium secondary battery; A positive electrode including a positive electrode active material; And electrolytes.
- the lithium salt that may be included as an electrolyte may be used, without limitation, those which are commonly used in a lithium secondary battery electrolyte, such as the lithium salt, the anion is F -, Cl -, Br - , I -, NO3 -, N (CN) 2 -, BF 4 -, ClO 4 -, PF 6 -, (CF 3) 2 PF 4 -, (CF 3) 3 PF 3 -, (CF 3) 4 PF 2 -, (CF 3) 5 PF -, (CF 3) 6 P -, CF 3 SO 3 -, CF 3 CF 2 SO 3 -, (CF 3 SO 2) 2N -, (FSO 2) 2 N -, CF 3 CF 2 (CF 3) 2 CO -, (CF 3 SO 2) 2 CH -, (SF 5) 3 C -, (CF 3 SO 2) 3 C -, CF 3 (CF 2) 7 SO 3 - , CF 3
- the lithium secondary battery of the present invention may be preferably used as a unit cell of a medium-large battery module including a plurality of battery cells, as well as a battery cell used as a power source for a small device such as a mobile phone.
- Applicable medium to large devices include a power tool; Electric vehicles including electric vehicles (EVs), hybrid electric vehicles (HEVs), and plug-in hybrid electric vehicles (PHEVs); Electric motorcycles including electric bicycles (Ebikes) and electric scooters (E-scooters); Electric Golf Carts; Electric trucks; Electric commercial vehicles; And a power storage system.
- a negative electrode mixture was prepared using the composition shown in Table 1 below using natural graphite as the carbon-based negative electrode active material, styrene-butadiene rubber as the binder, and PEDOT / PSS as the conductive polymer. Thereafter, the prepared negative electrode mixture was added to N-methylpyrrolidone to prepare a negative electrode active material slurry, which was then coated on a copper foil and dried at about 130 ° C. for 2 hours to prepare a negative electrode.
- the sheet resistance of the negative electrode manufactured by the composition of Synthesis Examples 1 and 2 was measured by using a surface resistance measuring instrument (4 point probe), which is shown in Table 2 below.
- a coin-type half cell was manufactured in a helium-filled glove box by using the negative electrode prepared in Synthesis Example 1 prepared above, a lithium counter electrode, a microporous polyethylene separator, and an electrolyte.
- the electrolyte 1 M LiPF 6 was dissolved in a solvent in which ethylene carbonate and dimethyl carbonate were mixed at a volume ratio of 50:50.
- a coin-type half cell (2016 R-type half cell) was manufactured in the same manner as in Example 1, except that the cathode prepared in Synthesis Example 2 was used.
- Example 1 The half-cells prepared in Example 1 and Comparative Example 1 were subjected to 50 cycles of charge / discharge at 0.5 C at 0 V to 1.5 V, and the change in the Coulomb effect and the charging capacity was measured. The results are shown in Figs. 2 (a) and 2 (b).
- the battery of Example 1 maintains 98% or more of initial capacity change even after 50 cycles, whereas the variation of charging capacity of the battery of Comparative Example 1 drops to 97% or less. In this respect, it can be seen that the life of the battery of Example 1 is improved.
- the life characteristics of the lithium ion battery according to the present invention are superior to those of the prior art, and can be rapidly charged at a high charge / discharge rate.
- the internal resistance of the battery was measured while the half cells prepared in Example 1 and Comparative Example 1 were subjected to high rate discharge at 5 C at 0 V to 1.5 V. The result is shown in FIG.
- Example 1 had a resistance characteristic lower than about 8 compared to the battery of Comparative Example 1.
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Abstract
Description
천연흑연(중량%) | SBR(중량%) | PEDOT/PSS (중량%) | |
합성예 1 | 93 | 6 | 1 |
합성예 2 | 92 | 5 | 0 |
음극 | 면저항(mΩ/m2) |
합성예 1 | 46.9 |
합성예 2 | 16.1 |
Claims (13)
- 카본계 음극 활물질, 바인더 및 전도성 고분자를 포함하는 리튬 이차전지용 음극에 있어서,상기 전도성 고분자는 화이버 형태를 갖는 것을 특징으로 하는 리튬 이차전지용 음극.
- 청구항 1에 있어서,상기 전도성 고분자는 PEDOT/PSS 인 것을 특징으로 하는 리튬 이차전지용 음극.
- 청구항 1에 있어서,상기 전도성 고분자는 음극 중의 고형분에 대하여 0.1~ 3 중량%로 포함되는 것을 특징으로 하는 리튬 이차전지용 음극.
- 청구항 1에 있어서,상기 전도성 고분자는 음극 중의 고형분에 대하여 0.5~ 2 중량%로 포함되는 것을 특징으로 하는 리튬 이차전지용 음극.
- 청구항 1에 있어서,상기 전도성 고분자는 음극 중의 고형분에 대하여 0.8~ 1.5 중량%로 포함되는 것을 특징으로 하는 리튬 이차전지용 음극.
- 청구항 1에 있어서,상기 바인더는 스티렌-부타디엔 고무, 니트릴-부타디엔 고무, (메트)아크릴산메틸-부타디엔 고무, 클로로프렌 고무, 카르복시 변성 스티렌-부타디엔 러버, 카르복시 메틸셀룰로스(CMC) 및 변성 폴리오가노실록산계 중합체로 이루어지는 군에서 선택되는 어느 하나 또는 2이상의 혼합물인 것을 특징으로 하는 리튬 이차전지용 음극.
- 청구항 1에 있어서,상기 카본계 음극 활물질은 연화탄소(soft carbon), 경화탄소(hard carbon), 천연 흑연, 키시흑연(Kish graphite), 열분해 탄소(pyrolytic carbon), 액정 피치계 탄소섬유(mesophase pitch based carbon fiber), 탄소 미소구체(meso-carbon microbeads), 액정피치(Mesophase pitches) 및 석유와 석탄계 코크스(petroleum or coal tar pitch derived cokes)으로 이루어지는 군에서 선택되는 어느 하나 또는 2이상의 혼합물인 것을 특징으로 하는 리튬 이차전지용 음극.
- (A) 카본계 음극 활물질 및 전도성 고분자를 바인더가 용해된 용액에 분산시켜 슬러리를 준비하는 단계;(B) 상기 슬러리를 음극활물질층이 형성된 집전체의 표면에 도포하는 단계; 및(C) 상기 (B) 단계에서 도포된 집전체를 건조시키는 단계를 포함하는, 청구항 1 의 리튬 이차전지용 음극의 제조방법.
- 청구항 8에 있어서,상기 전도성 고분자는 PEDOT/PSS 인 것을 특징으로 하는 리튬 이차전지용 음극의 제조방법.
- 청구항 8에 있어서,상기 전도성 고분자는 음극 중의 고형분에 대하여 0.1~ 3 중량%로 포함되는 것을 특징으로 하는 리튬 이차전지용 음극의 제조방법.
- 청구항 8에 있어서,상기 전도성 고분자는 음극 중의 고형분에 대하여 0.5~ 2 중량%로 포함되는 것을 특징으로 하는 리튬 이차전지용 음극의 제조방법.
- 청구항 8에 있어서,상기 전도성 고분자는 음극 중의 고형분에 대하여 0.8~ 1.5 중량%로 포함되는 것을 특징으로 하는 리튬 이차전지용 음극의 제조방법.
- 양극, 음극 및 전해질을 포함하는 리튬 이차전지에 있어서,상기 음극은 청구항 1 내지 청구항 7 중 어느 한 항의 음극인 것을 특징으로 하는 리튬 이차전지.
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JP2015552595A JP2016504739A (ja) | 2013-04-08 | 2014-02-07 | リチウム二次電池用負極、その製造方法、及びこれを含むリチウム二次電池 |
US14/761,704 US9601777B2 (en) | 2013-04-08 | 2014-02-07 | Anode for lithium secondary battery, method for manufacturing same, and lithium secondary battery including same |
EP14782986.5A EP2985818B1 (en) | 2013-04-08 | 2014-02-07 | Anode for lithium secondary battery, method for manufacturing same, and lithium secondary battery including same |
CN201480011795.4A CN105009331A (zh) | 2013-04-08 | 2014-02-07 | 锂二次电池用负极、其制造方法和包含其的锂二次电池 |
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KR20130038169A KR20140121953A (ko) | 2013-04-08 | 2013-04-08 | 리튬 이차전지용 음극, 그 제조방법 및 이를 포함하는 리튬 이차 전지 |
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CN105428083A (zh) * | 2015-12-30 | 2016-03-23 | 益阳市万京源电子有限公司 | 一种具备高导电率高机械强度的电极浆料 |
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US9601777B2 (en) | 2017-03-21 |
EP2985818B1 (en) | 2017-10-18 |
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US20150364766A1 (en) | 2015-12-17 |
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