KR100475697B1 - Manufacturing method of rechargeable lithium secondary battery - Google Patents

Manufacturing method of rechargeable lithium secondary battery Download PDF

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KR100475697B1
KR100475697B1 KR1019980002131A KR19980002131A KR100475697B1 KR 100475697 B1 KR100475697 B1 KR 100475697B1 KR 1019980002131 A KR1019980002131 A KR 1019980002131A KR 19980002131 A KR19980002131 A KR 19980002131A KR 100475697 B1 KR100475697 B1 KR 100475697B1
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electrode plate
secondary battery
lithium secondary
negative electrode
manufacturing
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KR1019980002131A
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Korean (ko)
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KR19990066306A (en
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최상훈
임대우
김순식
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주식회사 새 한
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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
    • 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
    • H01M10/058—Construction or manufacture
    • H01M10/0587—Construction or manufacture of accumulators having only wound construction elements, i.e. wound positive electrodes, wound negative electrodes and wound separators
    • 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
    • H01M4/36—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
    • 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
    • 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

Abstract

본 발명은 근래들어 새로운 전지로 각광을 받고 있는 충전용 리튬 2차전지의 제조방법에 관한 것으로서, 기존의 방법에 의해 제조된 리튬 2차전지 보다 수명이나 성능을 향상시키기 위해 안출된 것이다.BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a method for manufacturing a rechargeable lithium secondary battery, which has recently been spotlighted as a new battery, and has been devised to improve life and performance than a lithium secondary battery manufactured by a conventional method.

본 발명은 구체적으로 양극활물질(1)과 집전체(2)로 구성된 양극판과 음극활물질(3)과 집전체(2)로 구성된 음극판에 고분자 전해질(4)을 코팅한 후 코팅된 양극판과 음극판 사이에 플라스틱 재질의 세퍼레이터(5)를 넣고 적층시켜 제조한 단위 셀을 와인딩하여 제조하는 것을 특징으로 하는 충전용 리튬 2차전지의 제조법에 관한 것으로서, 이와 같이 제조함에 의해 수명이 크게 향상되는 등의 성능 향상을 도모할 수 있다.The present invention specifically covers the positive electrode plate (1) and the current collector (2) between the positive electrode plate and the negative electrode plate after coating the polymer electrolyte (4) on the negative electrode plate consisting of the negative electrode active material (3) and the current collector (2) The present invention relates to a method for manufacturing a rechargeable lithium secondary battery, which is manufactured by winding a unit cell manufactured by laminating a separator 5 made of plastic in a stack. Improvement can be aimed at.

Description

충전용 리튬 2차전지의 제조방법 Manufacturing method of rechargeable lithium secondary battery

본 발명은 충전용 리튬 2차전지의 제조방법에 관한 것으로서, 특히 양극판과 음극판 사이에 세퍼레이터를 넣고 적층시켜 제조함에 의해 전지의 성능을 향상시키는 방법에 관한 것이다.The present invention relates to a method of manufacturing a rechargeable lithium secondary battery, and more particularly, to a method of improving performance of a battery by inserting and stacking a separator between a positive electrode plate and a negative electrode plate.

리튬 고분자 전지는 양극과 음극, 그리고 고분자 전해질의 열을 가한 롤을 통과하면서 적층하는 것으로 알려져 있다. 또한, 리튬 고분자 전지는 이온 전지보다 안전성면에서 월등한 우위를 가지고 있는 것으로서, 이러한 고분자 전지를 제조하는 방법에 대한 여러 제안들이 알려져 있다.Lithium polymer batteries are known to be laminated while passing through rolls that are heated with a positive electrode, a negative electrode, and a polymer electrolyte. In addition, lithium polymer batteries have superior safety in terms of ion batteries, and various proposals for manufacturing such polymer batteries are known.

예를 들어, 각각의 전극(양극과 음극) 제조시에 리튬염을 함유한 상태에서 슬러리를 만들어 코팅 건조한 후, 역시 필름 형태로 제조된 리튬염을 함유하는 고체 전해질을 사이에 두고 열을 가한 롤을 통과시키면서 적층하는 방법이 있으며, 또한 리튬염을 함유하지 않은 상태로 각각 전극의 슬러리를 만들어 코팅 건조한 후, 마찬가지로 리튬염을 함유하지 않은 고체 전해질을 사이에 두고 적층한 후, 적층된 셀은 추출액에 의해 가소제 부분을 추출하고 액체액에 담근 후 건조시키는 제조공정이 알려져 있는데, 이러한 공정들은 미국특허 5,456,000과 5,470,357에 상세히 설명되어 있다.For example, a roll made of slurry in the state of containing lithium salt at the time of manufacture of each electrode (anode and cathode), coated and dried, and then heated with a solid electrolyte containing lithium salt, also manufactured in the form of a film, in between There is also a method of laminating while passing through, and after forming a slurry of the electrode in the state that does not contain lithium salt, coating and drying, and after laminating a solid electrolyte containing no lithium salt in between, the stacked cells are extracted liquid There is known a manufacturing process for extracting the plasticizer portion by immersion in a liquid liquid and then drying, which are described in detail in US Pat. Nos. 5,456,000 and 5,470,357.

이외에도 전극과 고체전해질과의 계면저항을 줄이면서, 전지 성능을 향상시킬 수 있는 여러 가지의 방법들이 연구되고 있다. 그러나, 상기 방법들은 성능이나 수명등에서 그리 만족할 만한 수준에는 이르지 못하고 있는 실정이다.In addition, various methods for improving battery performance while reducing interfacial resistance between electrodes and solid electrolytes have been studied. However, these methods do not reach a satisfactory level in performance or lifespan.

본 발명은 공정상의 효율을 높이고 전극과 전해질 사이에서의 계면저항을 줄임에 의해 성능이나 수명등이 우수한 리튬 2차전지의 제조법을 제공하는 것을 그 목적으로 한 것이다.It is an object of the present invention to provide a method for producing a lithium secondary battery which is excellent in performance and lifespan by increasing process efficiency and reducing interfacial resistance between an electrode and an electrolyte.

본 발명은 양극판과 음극판에 고분자 전해질을 코팅하는 공정과 상기 코팅된 양극판과 음극판 사이에 세퍼레이터를 라미네이팅하는 공정을 거쳐 만들어지는 양극판/세퍼레이터/음극판의 적층된 단위셀을 와인딩하여 제조하는 것을 특징으로 하는 충전용 리튬 2차전지에 관한 것이다.The present invention is prepared by winding a laminated unit cell of a positive electrode plate / separator / negative electrode plate made by a process of coating a polymer electrolyte on the positive electrode plate and the negative electrode plate and laminating the separator between the coated positive electrode plate and the negative electrode plate It relates to a rechargeable lithium secondary battery.

이하에서 첨부된 도면에 의거 본 발명을 구체적으로 설명한다.Hereinafter, the present invention will be described in detail with reference to the accompanying drawings.

본 발명에서 리튬 2차전지의 양극판은 양극활물질(1)과 집전체(2)로 구성되고, 음극판은 음극활물질(3)과 집전체(2)로 구성되는데, 양극활물질로는 LiMO2(여기서 M은 Co, Ni, Mn 등의 금속), LiMn2O4, Li(Ni0.5 Co0.5)O2 등이 단독 또는 혼합하여 사용될 수 있으며, 음극활물질로는 흑연 등의 탄소질 재료가 사용된다.In the present invention, the positive electrode plate of the lithium secondary battery is composed of the positive electrode active material (1) and the current collector (2), the negative electrode plate is composed of the negative electrode active material (3) and the current collector (2), as the positive electrode active material LiMO 2 (where M is a metal such as Co, Ni, Mn), LiMn 2 O 4 , Li (Ni 0.5 Co 0.5 ) O 2 and the like can be used alone or mixed, carbonaceous material such as graphite is used as the negative electrode active material.

그리고, 상기 활물질들의 코팅용 슬러리는 1몰 이하의 농도를 지닌 액체상태로 제공되고, 이들의 바인더로 사용가능한 고분자로는 PVdF 호모폴리머, PVdF 코폴리머, PVA, PVS, 우레탄아크릴레이트, PAN 등이 있으며, 용매로는 N-메틸피롤리돈(NMP), m-크레졸, 프로필렌카보네이트(PC) 등이 단독 또는 혼합되어 사용된다.In addition, the coating slurry of the active materials is provided in a liquid state having a concentration of 1 mol or less, and a polymer usable as a binder thereof includes PVdF homopolymer, PVdF copolymer, PVA, PVS, urethane acrylate, and PAN. As the solvent, N-methylpyrrolidone (NMP), m-cresol, propylene carbonate (PC) and the like are used alone or in combination.

본 발명에서는 상기와 같이 집전체(2)에 활물질 등의 코팅용 슬러리를 코팅하여 제조된 양극판(1)과 음극판(3)을 적층된 양극판과 음극판 사이에 폴리에틸렌, 폴리프로필렌 등의 플라스틱 물질로 만든 세퍼레이터(5)를 넣고 적층시켜 단위셀을 제조한다. 이때 극판의 코팅을 위해 사용되는 고분자 전해질(4)은 바인더로 활물질들의 코팅에 사용된 고분자 물질들을 사용하고, 용매로는 에틸렌 카보네이트, 프로필렌 카보네이트, 디메틸 카보네이트, 디에틸 카보네이트, 감마부티로락톤, 테트라-하이드로퓨란(THF), N-메틸피롤리돈(NMP), 아세토니트릴, 디메톡시에탄 등이 사용되며, 전해 물질로 LiClO4, LiPF6, LiAsF6, LiCF3SO3 등의 리튬염을 1몰 이하의 농도로 조절한 것으로서, 이온전도도가 10-2∼10-4S/m(Siemens/meter) 범위에 있도록 제조하여 사용한다.In the present invention, the positive electrode plate (1) and the negative electrode plate (3) prepared by coating a coating slurry such as an active material on the current collector (2) as described above is made of a plastic material such as polyethylene, polypropylene, etc. between the laminated positive plate and the negative plate The separator 5 is put in and laminated, and a unit cell is manufactured. At this time, the polymer electrolyte (4) used for the coating of the electrode plate is used as a binder polymer materials used for the coating of the active materials, the solvent is ethylene carbonate, propylene carbonate, dimethyl carbonate, diethyl carbonate, gamma butyrolactone, tetra -Hydrofuran (THF), N-methylpyrrolidone (NMP), acetonitrile, dimethoxyethane, etc. are used, and lithium salts such as LiClO 4 , LiPF 6 , LiAsF 6 , and LiCF 3 SO 3 are used as electrolytic materials. It is adjusted to a concentration of mole or less, and prepared and used so that the ion conductivity is in the range of 10 −2 to 10 −4 S / m (Siemens / meter).

이하에서 실시예 및 비교예를 들어 본 발명을 좀더 구체적으로 설명한다.Hereinafter, the present invention will be described in more detail with reference to Examples and Comparative Examples.

[실시예 1]Example 1

LiCoO2를 양극 활물질로 이용하고, 흑연을 음극 활물질로 사용하면서 바인더로는 PVdF 코폴리머, LiPF6 리튬염과 용매로 NMP를 이용하여 코팅 슬러리를 만들었다. 이렇게 만들어진 슬러리를 각각 알루미늄과 구리 박판위에 코팅하고(코팅두께 : 80㎛) 프레싱 하였다. 이후 200℃ 이상에서 건조된 극판은 0.5M의 농도를 가지는 고분자 전해질로 코팅하여 적층하였다. 이렇게 코팅된 전극판은 적어도 4시간 이상을 100℃ 이상의 대류오븐에서 건조하였다. 이어서, PE(폴리에틸렌)로 만들어진 세퍼레이터를 두 코팅된 극판 사이에 두고 라미네이션하여 400㎛ 두께의 단위셀을 제조하였다. 이 단위셀을 액체 전해질하에서 충방전 시험을 실시한 결과, 3.76V 정도의 초기방전전위를 나타냈으며, 수명은 50회 이상을 나타내었다.A coating slurry was prepared using LiCoO 2 as a positive electrode active material, graphite as a negative electrode active material, and a PVdF copolymer as a binder, LiPF 6 lithium salt, and NMP as a solvent. The slurry thus prepared was coated on aluminum and copper thin plates (coating thickness: 80 mu m) and pressed. Since the electrode plate dried at 200 ℃ or more was coated by laminating with a polymer electrolyte having a concentration of 0.5M. The coated electrode plate was dried in a convection oven of 100 ° C. or more for at least 4 hours. Subsequently, a separator made of PE (polyethylene) was placed between two coated electrode plates and laminated to prepare a unit cell having a thickness of 400 μm. As a result of the charge / discharge test under the liquid electrolyte, the unit cell exhibited an initial discharge potential of about 3.76 V and a lifetime of more than 50 times.

[비교예 1]Comparative Example 1

실시예 1에서 PE로 만들어진 세퍼레이터를 라미네이션 하는 공정을 실시하지 않은 것 외에는 실시예 1과 동일하게 실시하여 제조된 단위셀을 충방전 시험을 실시한 결과 초기방전전위는 3.76V 정도 이었고 수명은 28회 이었다.A charge and discharge test of the unit cell prepared in the same manner as in Example 1 was conducted except that the process of laminating the separator made of PE was performed in Example 1, and the initial discharge potential was about 3.76V and the lifetime was 28 times. .

상기 실시예 및 비교예에서도 확인되듯이 본 발명에 의해 세퍼레이터를 양극판과 음극판 사이에 넣고 적층시켜 제조된 단위셀을 기존의 단위셀에 비해 수명이 현저히 증대되는 장점을 지니기 때문에 충전용 리튬 2차전지로서 유용하다.As can be seen from the above examples and comparative examples, the rechargeable lithium secondary battery has a merit that the life of the unit cell manufactured by inserting and stacking the separator between the positive electrode plate and the negative electrode plate is significantly increased compared to the existing unit cell. Useful as

도 1은 본 발명에 따른 리튬 2차전지의 제조공정도.1 is a manufacturing process of the lithium secondary battery according to the present invention.

<도면의 주요부분에 대한 부호의 설명><Description of the symbols for the main parts of the drawings>

1 : 양극판 2 : 집전체1: positive electrode 2: current collector

3 : 음극판 4 : 고분자 전해질3: negative electrode plate 4: polymer electrolyte

5 : 세퍼레이터5: separator

Claims (2)

LiCoO2, LiNiO2, LiMnO2, LiMn2O4, Li(Ni0.5 Co0.5)O2 중에서 선택된 단독 또는 혼합의 양극활물질(1)과 집전체(2)로 구성되는 양극판과 흑연 또는 기타 탄소질 재료로 된 음극활물질(3)과 집전체(2)로 구성되는 음극판에 LiClO4, LiPF6, LiAsF6, LiCF3SO3 등의 리튬염을 1몰 이하의 농도로 함유하고 이온전도도가 10-2∼10-4S/m 범위에 있는 고분자 전해질(4)을 코팅한 후 상기 코팅된 양극판과 음극판 사이에 플라스틱 재질의 세퍼레이터(5)를 넣고 적층시켜 제조된 단위셀을 와인딩하는 것을 특징으로 하는 충전용 리튬 2차전지의 제조방법.A positive electrode plate and graphite or other carbonaceous material composed of a positive electrode active material (1) and a current collector (2), either alone or mixed, selected from LiCoO 2 , LiNiO 2 , LiMnO 2 , LiMn 2 O 4 , and Li (Ni 0.5 Co 0.5 ) O 2 It is the negative electrode plate consisting of a material the negative electrode active material (3) and the collector (2) containing a lithium salt such as LiClO 4, LiPF 6, LiAsF 6 , LiCF 3 SO 3 in a concentration of up to 1 mol of ionic conductivity 10 - After coating the polymer electrolyte (4) in the range of 2 ~ 10 -4 S / m after the separator (5) made of plastic material between the coated positive electrode plate and the negative electrode plate is laminated Method of manufacturing a rechargeable lithium secondary battery. 제 1 항에 있어서, 세퍼레이터는 폴리에틸렌 또는 폴리프로필렌을 재질로 하여 제조된 것임을 특징으로 하는 충전용 리튬 2차전지의 제조방법.The method of manufacturing a rechargeable lithium secondary battery according to claim 1, wherein the separator is made of polyethylene or polypropylene.
KR1019980002131A 1998-01-23 1998-01-23 Manufacturing method of rechargeable lithium secondary battery KR100475697B1 (en)

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US5219679A (en) * 1991-01-17 1993-06-15 Eic Laboratories, Inc. Solid electrolytes
KR970018824A (en) * 1995-09-20 1997-04-30 이정성 Copolymer Polymer Electrolyte in Lithium Secondary Battery
KR970018825A (en) * 1995-09-20 1997-04-30 이정성 Polymer Electrolyte in Lithium Secondary Battery
KR19980061921A (en) * 1996-12-31 1998-10-07 윤덕용 Polymer electrolyte composition comprising ionomer

Patent Citations (4)

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Publication number Priority date Publication date Assignee Title
US5219679A (en) * 1991-01-17 1993-06-15 Eic Laboratories, Inc. Solid electrolytes
KR970018824A (en) * 1995-09-20 1997-04-30 이정성 Copolymer Polymer Electrolyte in Lithium Secondary Battery
KR970018825A (en) * 1995-09-20 1997-04-30 이정성 Polymer Electrolyte in Lithium Secondary Battery
KR19980061921A (en) * 1996-12-31 1998-10-07 윤덕용 Polymer electrolyte composition comprising ionomer

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