JP5172234B2 - 過充電及び高温安全性に優れた電気化学素子 - Google Patents
過充電及び高温安全性に優れた電気化学素子 Download PDFInfo
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- JP5172234B2 JP5172234B2 JP2007196448A JP2007196448A JP5172234B2 JP 5172234 B2 JP5172234 B2 JP 5172234B2 JP 2007196448 A JP2007196448 A JP 2007196448A JP 2007196448 A JP2007196448 A JP 2007196448A JP 5172234 B2 JP5172234 B2 JP 5172234B2
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Description
本発明によるガス放出部材を構成するシェル成分は、素子の正常作動領域において電気化学的に安定した物性を有するだけでなく、コア表面の全体を均一に取り囲みうる高分子を用いることができる。このような高分子は接着力に優れているので、素子の内部空間に持続的に結着することもできる。
本発明によるガス放出部材における前記コア物質及び高分子シェルの重量比(%)は、1〜40:99〜60の範囲であることが好ましいが、これに制限されない。コアの含量が低すぎる場合、コアに含有されているガス放出物質の量が少なくなって電気化学素子の安全性を高める効果があまり得られなくなる。また、シェルの含量が低すぎる場合、コア−シェル構造が形成され難い。
本発明は、上述したガス放出部材が素子の内部空隙に取り込まれる電気化学素子を提供する。
1)第1の実施形態は、コア−シェル構造のガス放出部材を巻芯若しくはセンターピンの内部空間に挿入することであり、巻芯若しくはセンターピンを用いる電気化学素子に適用することが可能である。
前記ガス放出部材は、巻芯若しくはセンターピンの内部空間の100体積%まで取り込むことができる。しかしながら、温度変化に伴う体積の増大を考慮して、巻芯の内部空隙の10〜80%の範囲で充填されることが好ましい。このとき、ガス放出部材を巻芯若しくはセンターピンの内部に挿入する方法には特に制限はない。
2)第2の実施形態は、コア−シェル構造のガス放出部材を電解液に混合したり、バインダーを用いて電極の構成部分としたり、セパレーターの表面上に塗布したりして用いることである。
3)第3の実施形態は、素子用のケースの一部または全部にガス発生部材を塗布することである。この好適な一実施例を挙げると、粒状のガス発生部材が含有された塗布液に素子用のケースを含浸させ、あるいは、当業界における通常の方法に従い塗布した後に乾燥させて製造することである。
本発明による電気化学素子は、上述したガス放出部材と連動して素子の安全性を高める安全手段を備えることができる。
1−1.ガス放出部材の製造
高分子シェルは、ポリプロピレン製のものであって、ストロー状をなしている。前記高分子シェルの一方の先端を熱融着により封止した後、特定の温度ガス放出物質として下記式1で表されるアゾ系の化合物である2,2‘−アゾビス(2−シアノブタン)化合物0.4gを内部に仕込み、この後、他方の先端を熱融着させてガス放出部材を製造した。このとき、ガス放出部材の大きさは、最大 センターピンに合わせて製作した。製造されたガス放出部材の構造は、図1(a)に示すとおりである。
電池の巻芯部には、前記実施例1−1に従い製造されたカプセル型ガス放出部材を挿入した。
炭素粉体とポリビニリデンフルオライド(PVDF)バインダー、導電剤を92:4:4の重量比で混合した後、N‐メチル-2-ピロリドン(NMP)に分散させて負極混合物スラリーを製造した。この負極混合物スラリーを負極集電体として厚さ10μmの銅箔の単面にコンマギャップを200μmにして満遍なく塗布して乾燥した。このとき、塗布速度は3m/分であった。
特定の温度ガス放出物質として、2,2‘−アゾビス(2−シアノブタン)化合物に代えて、化学式2で表されるベンゾイルペルオキシド(BPO)0.4gを用いた以外は、前記実施例1の方法と同様にしてガス放出部材、巻芯及びリチウム二次電池をそれぞれ製造した。
ガス放出部材を使用せずに通常の方法に従い製造した以外は、前記実施例1の方法と同様にしてリチウム二次電池を製造した。
ガス発生物質である2,2‘−アゾビス(2−シアノブタン)を直接的に電解液に仕込んで製造した以外は、前記実施例1の方法と同様にしてリチウム二次電池を製造した。
2,2‘−アゾビス(2−シアノブタン)に代えて、ベンゾイルペルオキシド(BPO)を直接的に電解液に仕込んで製造した以外は、前記実施例1の方法と同様にしてリチウム二次電池を製造した。
本発明によるガス発生物質の電気化学的な安定性を下記のようにして評価した。
本発明によるガス発生物質の温度によるガス発生量を測定した。
巻芯部にガス放出部材が挿入された実施例1のリチウム二次電池を用い、通常の方法に従い製造された比較例1の電池を対照群とした。
実施例2と比較例1の電池をそれぞれ定電流で4.2Vまで充電し、5℃/分の速度で150℃まで昇温させた後、1時間保持した。この後、圧力感応素子であるCIDの作動時間とCIDの作動時における電池の温度をそれぞれ測定した。このとき、150℃まで昇温後、電池の発火及び爆発の発生(event)有無とこの爆発の発生にかかる時間をそれぞれ測定した。
Claims (16)
- ガス放出部材と、電気化学素子内部の圧力変化を感知し、前記電気化学素子の充電を中止させ、又は充電状態から放電状態へと切り替える、第1の安全手段とを備えた電気化学素子であって、
前記ガス放出部材が、前記電気化学素子内部の空隙に配置されてなるか、或いは、前記電気化学素子を形成する構成要素として使用されてなるものであり、
(a)50℃以上200℃以下の温度において、酸素以外のガスを放出する化合物を含有してなるコア部と、
(b)前記化合物を収容し、且つ、前記コア部を取り囲む、高分子シェル部と、及び
(i)前記電気化学素子内部の圧力変化を感知し、前記電気化学素子の充電を中止させ、又は充電状態から放電状態へと切り替える、第1の安全手段とを備えてなるものであり、 前記ガス放出部材が、60以上200℃以下の範囲で前記コア部と前記高分子シェル部とからなるコア−シェル構造が崩れることによりガスを発生し、前記高分子シェルの外部に放出する物質である、電気化学素子。 - 前記高分子のガラス遷移温度(Tg)又は溶融温度(Tm)が、60以上200℃以下の範囲である、請求項1に記載の電気化学素子。
- 前記高分子が、(メタ)アクリレート系の化合物、(メタ)アクリロニトリル系の化合物、(メタ)アクリル酸系の化合物、(メタ)アクリルアミド系の化合物、スチレン系の化合物、ビニリデンクロライド、ハロゲン化ビニール系の化合物、ブタジエン系の化合物、エチレン系の化合物、アセトアルデヒド及びホルムアルデヒドよりなる群から選ばれる1種以上の単量体を用いて重合させたポリマーまたは共重合体である、請求項1に記載の電気化学素子。
- 前記酸素以外のガスを放出する化合物が、アゾ系の化合物、有機過酸化物、ヒドラジド系の化合物、カルバジド系の化合物、カーボネート系の化合物、ペルオキシド系の熱化合物よりなる群から選ばれる、請求項1に記載の電気化学素子。
- 前記ガス放出部材から放出されるガスが、不活性ガス、消火用のガス及び可燃性ガスよりなる群から選ばれる、請求項1に記載の電気化学素子。
- 前記不活性ガスが、N2、He、Ne、Ar、Kr及びXeよりなる群から選ばれ、
前記消火用のガスが、CO2、F2、Cl2及びBr2よりなる群から選ばれ、 前記可燃性ガスが、プロパン、水素、プロピレン、一酸化炭素、メタン、エタン及びエチレンよりなる群から選ばれる、請求項5に記載の電気化学素子。 - 前記電気化学素子内の空隙が、電気化学反応が起こらない空間であり、かつ、巻芯の内部、センターピンの内部、前記電気化学素子ケースの内部上端及び内部下端よりなる群から選ばれる、請求項1に記載の電気化学素子。
- 前記ガス放出部材が、前記電気化学素子内部の空隙100体積%に対して10%以上100%以下の範囲になるように配置されてなる、請求項1に記載の電気化学素子。
- 前記電気化学素子の正常作動温度以上の温度範囲において、前記ガス放出部材から放出される酸素以外のガスにより、前記電気化学素子内部の構成要素と酸素との接触が遮断される、請求項1に記載の電気化学素子。
- 前記電気化学素子の正常作動温度以上の温度範囲において、前記ガス放出部材から放出されるガスにより、前記電気化学素子内部に存在し或いは発生する可燃性ガスまたは助燃性ガスの濃度が爆発範囲外となるように調節されてなる、請求項1に記載の電気化学素子。
- (ii)前記電気化学素子内部の圧力変化を感知し、前記電気化学素子内部の蓄熱又はガスを外部に発散させる第2の安全手段をさらに備えてなる、請求項1に記載の電気化学素子。
- 前記第1の安全手段が、圧力感応素子である、請求項1に記載の電気化学素子。
- 前記第1の安全手段が、
(i)圧力感応部材と、
(ii)前記圧力感応部材から伝わる電流を伝達する導線と、及び
(iii)前記導線を通って伝わる電流に応じて、前記電気化学素子の充電を中止させ、又は、充電状態から放電状態へと切り替える部材とを備えてなる、請求項1に記載の電気化学素子。 - 前記第2の安全手段が、圧力開放弁である、請求項11に記載の電気化学素子。
- 前記電気化学素子の正常作動温度以上の温度範囲において、高分子から放出されたガスの噴出圧による体積膨張及び前記電気化学素子内部の圧力増加により、第1の安全手段と第2の安全手段の何れか一方または両方が作動する、請求項13に記載の電気化学素子。
- リチウム二次電池である、請求項1に記載の電気化学素子。
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US8685557B2 (en) | 2010-04-07 | 2014-04-01 | Medtronic, Inc. | Electrode assembly including mandrel having a removable portion |
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