KR20020071204A - 다성분계 복합 필름을 이용한 전기화학소자 - Google Patents
다성분계 복합 필름을 이용한 전기화학소자 Download PDFInfo
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- KR20020071204A KR20020071204A KR1020010011192A KR20010011192A KR20020071204A KR 20020071204 A KR20020071204 A KR 20020071204A KR 1020010011192 A KR1020010011192 A KR 1020010011192A KR 20010011192 A KR20010011192 A KR 20010011192A KR 20020071204 A KR20020071204 A KR 20020071204A
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- South Korea
- Prior art keywords
- film
- electrochemical device
- support layer
- separator
- polymer
- Prior art date
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- 238000001179 sorption measurement Methods 0.000 description 1
- 239000013589 supplement Substances 0.000 description 1
- 230000008961 swelling Effects 0.000 description 1
- 238000012360 testing method Methods 0.000 description 1
- 229910052720 vanadium Inorganic materials 0.000 description 1
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Abstract
Description
구 분 | 다성분계 복합 필름 | |
두께(㎛) | 지지층 | 17 |
겔화 고분자층 | 1 | |
기공 크기(㎛ ×㎛) | 지지층 | 0.3 ×0.1 |
겔화 고분자층 | 0.8 ×0.3 | |
통기도(초/100 cc) | 520 | |
계면 접착력(gf) | 160 | |
전해액 함침속도(초) | 9 |
Claims (30)
- 전기화학소자에 있어서,a) ⅰ) 순차적으로 양극; 분리막; 및 음극이 위치되는 풀셀(full cell);또는ⅱ) ㄱ) 순차적으로 양극; 분리막; 음극; 분리막; 및 양극이 위치되거나;또는ㄴ) 순차적으로 음극; 분리막; 양극; 분리막; 및 음극이 위치되는바이셀(bicell)이 기본단위인 복수 개의 전기화학 셀이 중첩되고,ⅲ) 각각의 중첩부는 분리 필름이 개재되며,b) 상기 각각의 분리막, 분리필름, 또는 이들 모두가ⅰ) 고분자 지지층(support layer) 필름; 및ⅱ) 상기 필름의 한 면 또는 양면에 형성되는 다공성 겔화 고분자층(gellable polymer layer)을 포함하고, 상기 ⅰ)성분인 지지층 필름과 ⅱ)성분인 다공성 겔화 고분자층은 계면없이 일체화되는 다성분계 복합 필름인전기화학소자.
- 제 1 항에 있어서,상기 a)ⅰ)의 풀셀 또는 a)ⅱ)의 바이셀의 각각의 양극이 양극 물질, 및 양극 전류집전체를 포함하는 전기화학소자.
- 제 2 항에 있어서,상기 양극 물질이 리튬망간산화물(lithiated manganese oxide), 리튬코발트산화물(lithiated cobalt oxide), 리튬니켈산화물(lithiated nickel oxide), 및 이들의 복합산화물로 이루어진 군으로부터 1 종 이상 선택되는 리튬흡장물질(lithium intercalation material)인 전기화학 소자.
- 제 2 항에 있어서,상기 양극 전류집전체가 알루미늄, 및 니켈로 이루어진 군으로부터 1 종 이상 선택되는 재질의 호일인 전기화학 소자.
- 제 1 항에 있어서,상기 a)ⅰ)의 풀셀 또는 a)ⅱ)의 바이셀의 각각의 음극이 음극 물질, 및 음극 전류집전체를 포함하는 전기화학소자.
- 제 5 항에 있어서,상기 음극 물질이 리튬금속, 리튬합금, 카본(carbon), 석유코크(petroleum coke), 활성화 카본(activated carbon), 그라파이트(graphite)로 이루어진 군으로부터 1 종 이상 선택되는 리튬흡장물질인 전기화학 소자.
- 제 5 항에 있어서,상기 음극 전류집전체가 구리, 금, 니켈, 은, 구리합금로 이루어진 군으로부터 1 종 이상 선택되는 재질의 호일인 전기화학 소자.
- 제 1 항에 있어서,상기 b)ⅰ)의 고분자 지지층 필름은 재질이 고밀도 폴리에틸렌(high density polyethylene), 저밀도 폴리에틸렌(low density polyethylene), 선형 저밀도 폴리에틸렌(linear low density polyethylene), 폴리프로필렌(polypropylene), 고결정성 폴리프로필렌(high crystalline polypropylene), 폴리에틸렌-프로필렌 공중합체 (polyethylene-propylene copolymer), 폴리에틸렌-부틸렌 공중합체(polyethylene-butylene copolymer), 폴리에틸렌-헥센 공중합체(polyethylene-hexene copolymer), 폴리에틸렌-옥텐 공중합체(polyethylene-octene copolymer), 폴리스티렌-부틸렌-스티렌 공중합체(polystyrene-butylene-styrene copolymer), 폴리스티렌-에틸렌-부틸렌-스티렌 공중합체(polystyrene-ethylene-butylene-styrene copolymer), 폴리스티렌(polystyrene), 폴리페닐렌 옥사이드(polyphenylene oxide), 폴리설폰 (polysulfone), 폴리카보네이트(polycarbonate), 폴리에스테르(polyester), 폴리아미드(polyamide), 폴리우레탄(polyurethane), 폴리아크릴레이트(polyacrylate), 폴리비닐리덴 클로라이드(polyvinylidene chloride), 폴리비닐리덴 플루오라이드 (polyvinylidene fluoride), 폴리실록산(polysiloxane), 폴리올레핀 아이오노머(polyolefin ionomer), 폴리메틸펜텐(polymethyl pentene), 하이드로제네이티드 올리고사이클로펜타디엔(hydrogenated oligocyclopentadiene; HOCP), 및 이들의 공중합체 또는 유도체로 이루어지는 군으로부터 1 종 이상 선택되는 전기화학소자.
- 제 8 항에 있어서,상기 고결정성 폴리프로필렌이 밀도 0.905 g/cc 이상, 용융 온도 164 ℃ 이상, 결정화 온도 125 ℃ 이상, 결정화도 50 % 이상, 아이소탁티시티(또는 펜타드 분율) 96 % 이상, 및 아탁틱 분율 5 % 미만인 조건 중에서 1 종 이상의 조건을 만족하는 전기화학소자.
- 제 1 항에 있어서,상기 b)ⅰ)의 고분자 지지층 필름이 블렌드 필름 또는 적층(laminate) 필름인 전기화학소자.
- 제 1 항에 있어서,상기 b)ⅱ)의 겔화 고분자층은 재질이 폴리비닐리덴 플루오라이드 (polyvinylidene fluoride), 폴리비닐리덴 플루오라이드-클로로트리플루오로에틸렌 공중합체(polyvinylidenefluoride-chlorotrifluoroethylene copolymer), 폴리비닐리덴 플루오라이드-헥사플루오로프로필렌 공중합체 (polyvinyliden fluoride-hexafluoropropylene copolymer), 폴리에틸렌 옥사이드 (polyethylene oxide), 폴리프로필렌 옥사이드(polypropylene oxide), 폴리부틸렌 옥사이드(polybutylene oxide), 폴리우레탄(polyurethane), 폴리아크릴로니트릴 (polyacrylonitrile), 폴리아크릴레이트(polyacrylate), 폴리메틸 메타크릴레이트(polymethyl methacrylate), 폴리아크릴산(polyacrylic acid), 폴리아미드(polyamide), 폴리아크릴아미드(polyacrylamide), 폴리비닐아세테이트 (polyvinylacetate), 폴리비닐피롤리돈(polyvinylpyrrolidone), 폴리테트라에틸렌 글리콜 디아크릴레이트(polytetraethylene glycol diacrylate), 폴리설폰(polysulfone), 폴리페닐렌옥사이드(polyphenylene oxide), 폴리카보네이트(polycarbonate), 폴리에스테르(polyester), 폴리비닐리덴 클로라이드(polyvinylidene chloride), 폴리실록산(polysiloxane), 폴리올레핀(polyolefin) 아이오노머(ionomer) 및 이들의 공중합체 또는 유도체로 이루어지는 군으로부터 1 종 이상 선택되는 전기화학소자.
- 제 1 항에 있어서,상기 b)ⅱ)의 겔화 고분자층이 LiSCN, LiClO4, LiCF3SO3, LiAsF6, LiN(CF3SO2)2, 및 LiBF4로 이루어지는 군으로부터 1 종 이상 선택되는 리튬염을 더욱 포함하는 전기화학소자.
- 제 1 항에 있어서,상기 겔화 고분자층이 실리카(SiO2), 산화티탄(TiO2), 알루미나(Al2O3), 산화마그네슘(MgO), 및 산화바륨(B2O3)으로 이루어진 군으로부터 1 종 이상 선택되는 다공성 무기입자를 더욱 포함하는 전기화학소자.
- 제 1 항에 있어서,상기 b)ⅰ)의 지지층 필름은 기공 크기가 0.001 내지 10 ㎛이고, 두께가 1 내지 50 ㎛이고, b)ⅱ)의 다공성 겔화 고분자층은 기공 크기가 최대 10 ㎛ 이고, 두께가 0.01 내지 25 ㎛인 전기화학소자.
- 제 1 항에 있어서,상기 b)의 다성분계 복합필름이ⅰ) 고분자 지지층 필름을 제공하는 단계;ⅱ) 겔화 고분자를 용매에 용해하여 겔화 고분자 용액을 제조하는 단계;ⅲ) 상기 ⅱ)단계의 겔화 고분자 용액으로부터 상기 ⅰ)단계의 지지층 필름의 한 면 또는 양면에 겔화 고분자층을 형성시켜 다층 필름을 제조하는단계; 및ⅳ) 상기 ⅲ)단계의 다층 필름을 연신한 후 열 고정하는 단계를 포함하는 방법으로 제조되는 필름인 전기화학소자.
- 제 15 항에 있어서,상기 ⅲ)단계의 겔화 고분자층의 형성은 상기 ⅱ)단계의 겔화 고분자 용액을 상기 ⅰ)단계의 지지층 필름의 한 면 또는 양면에 도포한 후 건조하여 실시되는 전기화학소자.
- 제 15 항에 있어서,상기 ⅲ)단계의 겔화 고분자층의 형성은 상기 ⅱ)단계의 겔화 고분자 용액을 이형 필름 위에 도포하고, 건조한 후 이형 필름에서 탈착시키고, 탈착된 필름을 상기 ⅰ)단계의 지지층 필름의 한 면 또는 양면에 열접착시켜 실시되는 전기화학소자.
- 제 16 항 또는 제 17 항에 있어서,상기 각각의 도포가 딥코팅(dip coating), 분사코팅(spray coating), 스핀코팅(spin coating), 다이코팅(die coating), 및 롤코팅(roll coating)으로 이루어진 코팅군으로부터 선택되는 방법으로 실시되는 전기화학소자.
- 제 16 항 또는 제 17 항에 있어서,상기 각각의 건조는 상대습도가 1 내지 100 %이고, 압력이 최대로 상기 겔화 고분자 용액 중의 용매의 포화 증기압이며, 및 질소, 산소, 이산화탄소 및 공기로 이루어진 군으로부터 1 종 이상 선택되는 가스의 분위기 하에서 실시되는 전기화학소자.
- 제 15 항에 있어서,상기 ⅳ)단계의 연신은 저온 연신한 후 고온 연신을 실시하는 전기화학소자.
- 제 20 항에 있어서,상기 저온 연신은 필름을 롤(roll) 또는 연신기에서 0 내지 50 ℃의 온도 조건 하에 1 축으로 연신시키는 전기화학소자.
- 제 20 항에 있어서,상기 고온 연신은 필름을 롤(roll) 또는 연신기에서 50 ℃ 내지 최대로 지지층 또는 겔화 고분자층의 고분자 용융점의 온도 조건 하에 1 축 또는 2 축 연신시키는 전기화학소자.
- 제 15 항에 있어서,상기 ⅳ)단계의 열 고정은 50 ℃ 내지 최대로 지지층 또는 겔화 고분자층의 고분자 용융점의 온도 조건 하에서 필름이 장력을 받은 상태로 10 초 내지 1 시간의 일정 시간 동안 고정하여 실시되는 전기화학소자.
- 제 15 항에 있어서,상기 ⅰ)단계의 지지층 필름이 고분자를 T-다이(T-die) 또는 원형 관다이(tubular die)가 부착된 압출기(extruder)에 투입하여 압출한 후, 건조 오븐에서 상온 내지 최대 지지층의 고분자 용융점의 온도 조건 하에 어닐링(annealing)시켜 제조되는 필름인 전기화학소자.
- 제 15 항에 있어서,상기 ⅰ)단계의 지지층 필름이 반응성 가스 분위기 하에 지지층 필름의 한 면 또는 양면에 이온 빔이 조사되어 제조되는 필름인 전기화학소자.
- 제 25 항에 있어서,상기 이온 빔 조사가 10-1내지 10-6torr의 진공도를 가지는 진공 조에서 헬륨, 수소, 산소, 질소, 암모니아, 일산화 탄소, 이산화 탄소, 사불화 탄소, 메탄, 및 N2O로 이루어진 군으로부터 1 종 이상 선택되는 반응성 가스를 0.5 내지 20 ㎖/분의 주입량으로 주입하여 조성되는 반응성 가스 분위기 하에 전자, 수소, 헬륨, 산소, 질소, 이산화탄소, 공기, 불소, 네온, 아르곤, 크립톤, 및 N2O로 이루어진 군으로부터 1 종 이상 선택되는 입자를 여기시켜 10-2내지 106keV의 에너지를 가지게 하여 생성된 이온 빔을 105내지 1020ions/cm2의 조사량으로 조사하는 전기화학소자.
- 제 15 항에 있어서,상기 ⅱ)단계의 용매가 1-메틸-2-피롤리돈(1-methyl-2pyrrolidone, NMP), 아세톤(acetone), 에탄올(ethanol), n-프로판올(n-propanol), n-부탄올(n-butanol), n-헥산(n-hexane), 사이클로헥산올(cyclohexanol), 아세틱 산(acetic acid), 에틸아세테이트(ethyl acetate), 디에틸에테르(diethyl ether), 디메틸포름아미드 (dimethyl formamide; DMF), 디메틸아세트아미드(dimethylacetamide; DMAc), 다이옥산(dioxane), 테트라하이드로퓨란(tetrahydrofuran; THF), 디메틸술폭사이드 (dimethyl sulfoxide; DMSO), 사이클로헥산(cyclohexane), 벤젠(benzene), 톨루엔 (toluene), 크실렌(xylene), 물(water), 및 이들의 유도체로 이루어진 군으로부터 1 종 이상 선택되는 전기화학소자.
- 제 15 항에 있어서,상기 ⅱ)단계의 겔화 고분자 용액의 농도가 0.01 내지 90 중량%인 전기화학소자.
- 제 1 항에 있어서,상기 전기화학소자가ⅰ) ㄱ) 다공성 지지층 필름; 및ㄴ) 상기 ㄱ)의 지지층 필름의 한 면 또는 양면에 형성되는 다공성 겔화고분자층을 포함하고, 상기 ㄱ)성분인 지지층 필름과 ㄴ)성분인 다공성 겔화 고분자층은 계면없이 일체화되는 다성분계 복합 필름의 분리막; 및ⅱ) ㄱ) 하기 화학식 1로 표시되는 염; 및ㄴ) 유기용매를 포함하는 액체 전해질을 포함하는 고분자 전해질 시스템을 포함하는 전기화학소자:[화학식 1]A+B-상기 식에서,A+는 Li+, Na+, 및 K+으로 이루어진 알칼리 금속 양이온군, 및 이들의 유도체로부터 1 종 이상 선택되며,B-는 PF6 -, BF4 -, Cl-, Br-, I-, Cl-, AsF6 -, CH3CO2 -, CF3SO3 -, N(CH3SO2)2 -, 및 C(CH3SO2)3 -으로 이루어진 군으로부터 1 종 이상 선택된다.
- 제 29 항에 있어서,상기 ⅱ)ㄴ)의 유기 용매가 프로필렌 카보네이트(propylene carbonate; PC), 에틸렌 카보네이트(ethylene carbonate; EC), 디에틸카보네이트(diethyl carbonate; DEC), 디메틸카보네이트(dimethyl carbonate; DMC), 디프로필카보네이트(dipropyl carbonate; DPC), 디메틸설폭사이드(dimethyl sulfoxide), 아세토니트릴(acetonitrile), 디메톡시에탄(dimethoxyethane), 디에톡시에탄(diethoxy ethane), 테트라하이드로퓨란(tetrahydrofuran), N-메틸-2-피롤리돈(N-methyl-2- pyrrolidone; NMP), 및 에틸메틸카보네이트(ethyl methyl carbonate; EMC)로 이루어진 군으로부터 1 종 이상 선택되는 전기화학소자.
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Also Published As
Publication number | Publication date |
---|---|
US7014948B2 (en) | 2006-03-21 |
EP1285468A4 (en) | 2004-07-21 |
CN1457517A (zh) | 2003-11-19 |
JP4204321B2 (ja) | 2009-01-07 |
EP1285468B1 (en) | 2006-06-14 |
WO2002071509A1 (en) | 2002-09-12 |
EP1285468A1 (en) | 2003-02-26 |
CN1274036C (zh) | 2006-09-06 |
DE60212274D1 (de) | 2006-07-27 |
JP2004519824A (ja) | 2004-07-02 |
US20030104273A1 (en) | 2003-06-05 |
KR100406690B1 (ko) | 2003-11-21 |
DE60212274T2 (de) | 2007-05-31 |
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