JP2007510267A - 高分子が独立的な相にコーティングされた電極及びこれを含む電気化学素子 - Google Patents
高分子が独立的な相にコーティングされた電極及びこれを含む電気化学素子 Download PDFInfo
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- JP2007510267A JP2007510267A JP2006537892A JP2006537892A JP2007510267A JP 2007510267 A JP2007510267 A JP 2007510267A JP 2006537892 A JP2006537892 A JP 2006537892A JP 2006537892 A JP2006537892 A JP 2006537892A JP 2007510267 A JP2007510267 A JP 2007510267A
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Abstract
Description
本発明者らは通常的な方法によって電極を製造した後、製造された電極を高分子溶液に含浸させることで、電極活物質粒子ら間の空間による気孔構造を維持しながら電極活物質の表面に独立的な相(phase)形態の高分子コーティング層が形成されることによって、従来技術で電極活物質粒子らの擬集及び高分子コーティング層の離脱などのような問題点を解決するだけでなく、電池の性能低下防止及び安全性の向上を示すということを明かした。
通常的な方法によって製造された電極は集電体上に電極活物質が望ましくは、バインダーによって固定及び連結されたものであり、本発明は前記のように製造された電極を高分子、望ましくは電解液によって膨潤及び/または可溶される電解液機能性高分子が含有された溶液に含浸させてコーティングすることを特徴とする。
電解液可溶性の高分子の濃度多様化による電解液の粘度及びイオン伝導度の変化を観察した。採択された電解液可溶性の高分子はシアノ−エチルプルランであったし、電解液は1MのLiPF6が溶解されたEC/PC/DEC=3/2/5(重量比)を選定した。シアノ−エチルプルランの電解液に対する濃度をそれぞれ0重量%、5重量%、10重量%で調節した。
実施例1
1-1.シアノ−エチルプルランがコーティングされた電極製造
正極活物質でリチウムコバルト複合酸化物94重量%、導電材でカーボンブラック(carbon black)3重量%、結合剤でPVDF3重量%を溶剤であるN-メチル-2ピロリドン(NMP)に添加して正極混合物スラリーを製造した。前記正極混合物スラリーを厚さが20μmである正極集電体であるアルミニウム(Al)薄膜に塗布、乾燥を実施して正極を製造した。
(負極の製造)
負極活物質で炭素粉末、結合材でポリビニリデンフルオライド(PVDF)、導電材でカーボンブラックをそれぞれ93重量%、6重量%、1重量%にして溶剤であるN-メチル-2ピロリドン(NMP)に添加して負極混合物スラリーを製造した。前記負極混合物スラリーを厚さが10μmである負極集電体である銅(Cu)薄膜に塗布、乾燥を通じて負極を製造した後ロールプレス(roll press)を実施した。
前記製造された正極、負極及びポリプロピレン/ポリエチレン/ポリプロピレン(PP/PE/PP)3層でなされた分離膜をスタッキング(stacking)方式で組立てた後、電解液(エチレンカーボネート(EC)/プロピレンカーボネート(PC)=50/50嵩%、1Mのリチウムヘキサフルオロホスファート(LiPF6))を入れ込んで最終的に電池を完成した。
高分子でシアノ−エチルプルランの代わりにシアノ−エチルポリビニルアルコールを使ったことを除き、前記実施例1と同一な方法で正極及び電池を製造した。
高分子でシアノ−エチルプルランの代わりにポリメチルメタクリレート(PMMA)を使ったことを除き、前記実施例1と同一な方法を遂行して正極及び電池を製造した。
シアノ−エチルプルランが両電極にすべて導入したことを除き、前記実施例1と同一な方法を遂行して両電極及び電池を製造した。
シアノ−エチルプルラン(重合度=約600)をアセトンにとかした後、PP/PE/PPの3層でなされた分離膜の表面にディップコーティング(dip coating)方式で取り入れた。コーティング後に常温乾燥及び100℃熱風乾燥を通じて最終製品を製造したし、分離膜の表面にコーティングされた高分子コーティング層の厚さは約1μmであった。
高分子でシアノ−エチルプルランの代わりにポリエチレングリコールジメチルエーテル(分子量1,000)を使ったことを除き、前記実施例5と同一な方法を遂行して電池を製造した。
電極に高分子が導入されないことを除き、前記実施例1と同一な方法を遂行して電極及びリチウム二次電池を製造した。
本発明によって高分子がコーティングされた電極内の電極活物質の表面を分析するため、下記のように実施した。
実施例1ないし6及び比較例1のリチウム二次電池の熱的安全性を評価するために、下記のように実施した。
実施例1ないし6及び比較例1のリチウム二次電池の性能を評価するために各電池の容量及びC-Rateを測定した。
下記の特許請求の範囲に記載した本発明の思想及び領域から脱しない範囲内で本発明を多様に修正及び変更させることができる。したがって特許請求範囲の等価的な意味や範囲に属するすべての変化らは全部本発明の権利範囲内に属することを明らかにしておく。
Claims (18)
- 集電体上に電極活物質を含む電極において、前記電極はお互いに連結された状態の電極活物質の表面が高分子によってコーティングされた電極であって、高分子はお互いに連結された状態の電極活物質粒子らの間に形成された気孔構造をそのまま維持しながら独立的な相(phase)で存在することを特徴とする電極。
- 前記高分子は誘電率常数(測定周波数=1kHz)が1.0ないし100の範囲であることを特徴とする請求項1に記載の電極。
- 前記高分子は使おうとする電解液によって可溶性、膨潤(swelling)性、不溶性またはこれらの混合物性であることを特徴とする請求項1に記載の電極。
- 前記電解液可溶性及び電解液膨潤性の高分子は溶解度指数(solubility parameter)が18.0ないし30[J1/2/cm3/2]範囲である請求項3に記載の電極。
- 前記電解液膨潤性の高分子はポリエチレンオキサイド、ポリビニリデンフルオライド-ヘキサフルオロプロピレン、ポリビニリデンフルオライド-トリクロロエチレン、ポリメチルメタクリレート、ポリアクリロニトリル、ポリアクリロニトリル-スチレン共重合体、ポリ塩化ビニル(PVC)、ポリビニルピロリドン、ポリビニルアセテート、ポリエチレンビニルアセテート共重合体及びゼラチンでなされた群から選択された1種以上である請求項3に記載の電極。
- 前記電解液可溶性の高分子はシアノ−エチルプルラン、シアノ−エチルポリビニルアルコール、シアノエチルセルロース、シアノ−エチルスクロース、プルラン、セルロースアセテート、セルロースアセテートブチレート、セルロースアセテートプロピオネート、ポリエチレングリコール、グリム、ポリエチレングリコールジメチルエーテル及びポリピロリドンでなされた群から選択された1種以上である請求項3に記載の電極。
- 前記高分子コーティング層の厚さは1nmないし1μm範囲である請求項1に記載の電極。
- 前記電極の気孔度は1ないし50%範囲である請求項1に記載の電極。
- 正極、負極、両電極との間に介された分離膜及び電解液を含む電気化学素子において、前記正極、負極または両電極はお互いに連結された状態の電極活物質粒子らの間に形成された気孔構造をそのまま維持しながら電極活物質の表面にコーティングされた高分子が独立的な相(phase)で存在する電極であることを特徴とする電気化学素子。
- 前記電気化学素子はリチウム二次電池である請求項9に記載の電気化学素子。
- 前記電解液は下記一般式(I)で表記する塩がプロピレンカーボネート(PC)、エチレンカーボネート(EC)、ジエチルカーボネート(DEC)、ジメチルカーボネート(DMC)、ジプロピルカーボネート(DPC)、ジメチルスルホキシド、アセトニトリル、ジメトキシエタン、ジエトキシエタン、テトラヒドロフラン、N-メチル-2-ピロリドン(NMP)、エチルメチルカーボネート(EMC)及びガンマブチロラクトンでなされた群から選択された1種以上の有機溶媒に解離されたことを特徴とする請求項9に記載の電気化学素子:
A+B-(I)
前記式において、A+はアルカリ金属陽イオンまたはこれらの組合でなされたイオンを含んで、B-は陰イオンまたはこれらの組合でなされたイオンを含む。 - 前記電極活物質の表面に独立的な相でコーティングされた高分子は電解液の注入によって電解液溶媒を含んで膨潤するか、及び/または電解液注入によって溶解されて電解質を形成することを特徴とする請求項9に記載の電気化学素子。
- 前記電極活物質の表面に独立的な相でコーティングされた高分子が電解液注入によって含む電解液溶媒量は0.1ないし20重量%範囲である請求項12に記載の電気化学素子。
- 前記電極活物質の表面に独立的な相でコーティングされた高分子が電解液注入によって溶解されて形成された電解質は電気化学素子導入前の電解液造成に比べて0.01ないし20重量%範囲の高分子を含むことを特徴とする請求項12に記載の電気化学素子。
- 前記電極活物質の表面に独立的な相でコーティングされた高分子が電解液注入によって溶解されて形成された電解質は電気化学素子の両電極の表面、電極活物質の間または電極に存在する気孔部、分離膜の表面及び分離膜の気孔部に均一に浸透することを特徴とする請求項12に記載の電気化学素子。
- (a)電極活物質を含む電極スラリーを電流集電体に塗布及び乾燥して電極を製造する段階と、及び
(b)製造された電極(a)を高分子が溶解された溶液に含浸する段階と、
を含んでお互いに連結された電極活物質の表面に独立的な相(phase)形態の高分子コーティング層が形成されて、電極活物質粒子らの間に形成された気孔構造がそのまま維持されることを特徴とする電極の製造方法。 - 前記(b)段階でのコーティング方法はディップ(dip)コーティング、ダイ(die)コーティング、ロール(roll)コーティング、コンマ(comma)コーティングまたはこれらの混合方式でなされた群から選択されたことを特徴とする請求項16に記載の製造方法。
- (a)電極活物質を含む電極スラリーを集電体上に塗布及び乾燥して電極を製造した後、製造された電極を高分子が溶解された溶液に含浸させて電極活物質粒子らの間の気孔構造が維持されてお互いに連結された電極活物質の表面に独立的な相で高分子がコーティングされた電極と分離膜とを利用して組立てる段階と、;及び
(b)前記段階(a)で製造された組立体に電解液を入れ込む段階と、
を含む電気化学素子の製造方法。
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KR20050043674A (ko) | 2005-05-11 |
WO2005045957A1 (en) | 2005-05-19 |
CA2545174C (en) | 2015-05-19 |
EP1690307A1 (en) | 2006-08-16 |
EP1690307B1 (en) | 2014-03-05 |
TW200601603A (en) | 2006-01-01 |
EP1690307A4 (en) | 2009-09-02 |
JP4489778B2 (ja) | 2010-06-23 |
CA2545174A1 (en) | 2005-05-19 |
US7700226B2 (en) | 2010-04-20 |
TWI258238B (en) | 2006-07-11 |
US20050118508A1 (en) | 2005-06-02 |
KR100612572B1 (ko) | 2006-08-11 |
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