TWI416785B - 用於可充電電池之矽陽極 - Google Patents

用於可充電電池之矽陽極 Download PDF

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TWI416785B
TWI416785B TW097119460A TW97119460A TWI416785B TW I416785 B TWI416785 B TW I416785B TW 097119460 A TW097119460 A TW 097119460A TW 97119460 A TW97119460 A TW 97119460A TW I416785 B TWI416785 B TW I416785B
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Description

用於可充電電池之矽陽極
本發明關於用於可充電電池單元的一電極，其使用矽或矽基底材料作為其主動成分，其係特別用於鋰離子電池單元，但亦非排除其他用途。
近來可攜式電子裝置使用的增加，如行動電話與筆記型電腦，已創造出對於較小、較輕、持續性較長的可充電電池的需求，以提供該電源至上述及其他電池供電裝置。1990年代期間，可充電鋰電池(尤其是鋰離子電池)以銷售量看來變得很受歡迎，且現在在可攜式電子市場已成為主流。然而，隨著上述裝置加入越來越多的需電源功能(如行動電話上的相機)，需要每單元質量與每單元體積能儲存更多能量的改進電池。
眾所周知的，矽可用做為可充電鋰離子電化學電池單元的主動陽極材料(舉例來說，可見「用於可充電鋰電池之插入電極材料」M. Winter, J. O. Besenhard, M. E. Spahr,與P. Novuk於Adv. Mater. 1998, 10, No. 10)。傳統可充電鋰離子電池單元的基本組成係顯示於圖1，包含石墨基底陽極電極，該組成係由該矽基底陽極取代。該電池單元包含單一單元，但也可包含多於一個單元。
電池單元一般包含用於該陽極的銅電流收集器10，以及用於陰極的鋁電流收集器12，其可外部連接至一負載或 接至適宜的充電來源。一石墨基底複合陽極層14覆蓋該電流收集器10，且一含鋰金屬氧化物基底複合陰極層16係覆蓋該電流收集器12。多孔塑膠間隔物或分隔物20係提供於該石墨基底複合陽極層14與該含鋰金屬氧化物基底複合陰極層16之間，且液態電解材料係塗布於多孔塑膠間隔物或分隔物20、該複合陽極層14，與該複合陰極層16之中。一些例子中，該多孔塑膠間隔物或分隔物20可由聚合物電解材料所取代，且於此等例子中，該聚合物電解材料係同時於該複合陽極層14與該複合陰極層16之中。
當該電極單元完全充電，鋰已經經由該電解質自該含鋰金屬氧化物傳送至該石墨基底層中，於其中，鋰係與石墨反應以產生化合物LiC6 。該石墨係為該複合陽極層中的電化學主動材料，且具有最大電容為372 mAh/g。應注意「陽極」與「陰極」一詞係用以表示該電池係橫跨一負載而放置。
一般相信當矽用作為可充電鋰離子電池中的主動陽極材料，其所提供的電容大大高過目前使用的石墨。當矽藉由與電化學電池中的鋰反應來轉換為化合物Li21 Si5 ，其具有最大電容4,200 mAh/g，顯著地高過石墨的最大電容。因此，若在可充電鋰電池中的石墨可被矽取代，則可達到所希的每單元質量與每單元體積儲存能量的增加。
現有的於電化學鋰離子電池中使用矽或矽基底主動陽極材料的方法無法在所需的充/放電週期數量中表現維持的 電容，且因此無法商業化。
本發明中揭示的一種方法，其係利用粉末形式(如顆粒或直徑10μm的球型元件)的矽，在一些例子中係製成具有或沒有電子添加物的複合物，並包含一適合的黏結劑，如銅電流收集器上鍍的聚偏二氟乙烯。然而，此電極系統在重複實施充/放電週期時無法表現維持的電容。普遍相信此電容的損失是因為大量矽粉末的部分機械性隔絕，其係由於關於鋰插入至/抽出自該主體矽的體積膨脹/收縮。結果此會造成同時來自同電流收集器與自身的矽元件產生電性絕緣。此外，該體積膨脹/收縮造成該球型元件分散，其係造成該球型元件自身中的電性接觸的損失。
本發明另一種眾所周知的方法係設計以處理連續週期期間大量體積變化的問題，其係用以使形成矽粉末的矽元件的大小非常小，其係使用直徑在1-10nm範圍內的球型顆粒。此策略假設該等奈米尺度元件可歷經關於鋰插入/抽出的大量體積膨脹/收縮，而不會分散或毀壞。然而，此方法仍有其問題，即需要處理非常細、奈米尺度的粉末，其係造成健康與安全的風險，且在該矽粉末經歷關於鋰插入/抽出的體積膨脹/收縮時，其無法防止該球型元件使該銅電流收集器與其自身電性隔絕。重要地，由於包含鋰的表面膜一般係在鋰插入期間創出，且組成此表面膜的鋰離子被困住且無法在反插入(deinsertion)過程期間被移除，該奈米尺度元件的大表面區域可將大的不可反轉電容帶入該鋰電池單元中。此外，該等大量的小矽顆粒為固定量的矽 創造了大量的顆粒間接觸，且此等每一者具有一個接觸阻抗，且可因此使得該等矽的電性阻抗過高。該等上述問題因此使得矽顆粒無法成為在可充電鋰電池中的一個可商業化的石墨取代物，且特別指鋰離子電池。
由Ohara等人於電源期刊(Journal of Power Sources)136(2004)303-306中描述，矽係蒸鍍至一鎳箔電流收集器上作為一薄膜，且此結構係接著被用以形成鋰離子電池的陽極。然而，雖然此方法可有好的電容保持力，此僅為非常薄膜(如~50nm)的例子，且因此這些電極結構無法在每單位面積給予可用的電容量。膜厚度的增加(如>250nm)係造成好的電容維持力被削減。此等薄膜的好的電容維持力，現今發明者認為係由於薄膜吸收體積膨脹/收縮的能力所造成，其係關於自該主體矽的鋰插入/抽出，且該膜不會分散或毀壞。同時，該薄膜的表面面積較等量的奈米尺度顆粒少了許多，且因此由於包含鋰表面膜的形成所造成的不可逆電容量係減少。該等上述問題因此使得一金屬箔電流收集器上的矽薄膜無法成為在可充電鋰電池中的一個可商業化的石墨取代物，且特別指鋰離子電池。
US 6,887,511中描述的另一種方法，矽係蒸發至一粗糙的銅基板上以創造出上至約10μm的中厚度膜。在鋰離子插入製程開始期間，該矽膜係分散以形成多個矽柱。這些柱係接著與鋰離子進行可逆的反應，並可有好的電容維持力。然而，該製程無法以較厚的膜良好運作，且創造該中厚度膜為一昂貴的製程，因此限制了此概念的商業化可 行性。同時，由該膜分散所創造的柱狀結構並沒有固有的多孔性，因此長遠的電容維持性係可質疑的。
US2004/0126659中描述的另一種方法中，矽係蒸發至鎳纖維上，該等纖維係接著用以形成鋰電池的陽極。然而，已發現此係於鎳纖維上提供矽的不均勻分布，因此嚴重影響操作。此外，這些結構的鎳電流收集器與主動矽的質量比很高，且因此每單位面積或每單位質量不會有有用的電容量。
Kasavajjula等人已提供用於鋰離子第二電池的奈米與主體矽基底插入陽極的回顧(J. Power Sources (2006))，以參考文獻合併於本文中。
本發明係設定於獨立項的申請專利範圍中。
一些實施例占有優勢地提供一電極，其包含作為其主動材料的高縱寬比例的矽或矽基底元件的互連陣列。當該等元件的結構可符合關於矽或矽基底元件插入/抽出(充電及放電)的體積膨脹，且有最小尺度的上限，且該最小尺度的較低限制控制固定體積的矽或矽基底的表面面積比例，週期壽命係獲得改進，因此可使該關於表面的不可逆電容最小化。至少有一種其他的尺度係選定為足夠大，足以確保元件間的複數個接觸，以獲得良好的導電性。
該等高縱寬比元件可被延長，例如類似帶狀的，以此第一較大尺度係大於該最小尺度，且一第二較大尺度係大於該第一較大尺度。該等高縱寬比元件也可為類似薄板狀 的或類似薄片狀的，其中該等第一與第二較大尺度係大於該第一尺度，但彼此大小相同。
本發明會於本文中描述，僅藉由舉例與配合附圖1，圖示顯現一可充電鋰離子電池，其包含一根據本發明實施例的陽極。
發明者已知該等上述問題與先前技藝的缺點可藉由謹慎地選擇矽或矽基底元件的尺度以及形狀來解決，該等元件為用於一可充電電池之電極的主動成分。至於延長的元件，其具有兩個相同並小於第三尺度(稱為餘項中的纖維)的尺度，至一第一預估，該不可逆電容損失係反比於該纖維的尺度。類似地，對於延長的結構，兩個較小的尺度中的一個係大於另一個，舉例來說，係為較小尺度的兩倍或更大(下面稱為帶狀)，且對於有兩個相同最大尺度與單一較其(稱為薄板或薄片)為小的尺度的元件來說，該不可逆電容可顯示為大略反比於該帶狀或薄片的厚度(即為最小尺度)，忽略該帶狀或薄板的側邊。因此，對於纖維、帶狀、薄片，或薄板，最小尺度十倍的減少係可預料會造成不可逆電容損失有十倍的增加。這些考量係把一較低限制加於這些結構的最小尺度上，若其係用以作為具有受限的不可逆電容損失的複合電極中的矽元件。
如上所述，使用矽或矽基底材料作為可充電鋰離子電池主動陽極材料的一個嚴重問題為體積係大量改變，其係關於該電池的充電與放電。該相關應力導致主體矽中形成裂縫，如上所述。柱狀矽基板的實驗實作顯示出接近直徑 1微米(約0.8微米)的矽柱可被形成，其可順應該體積改變而不會有裂縫【Mino Green, Elizabeth Fielder, Bruno Scrosati, Mario Wachtler與Judith Serra Moreno,「用於鋰電池應用的結構性矽陽極」,Electrochemical and Solid-State Letter: 6,A75-A79 (2003)】。更進一步，矽板上的實驗實作已顯示即使在厚板(350微米厚)應力破斷具有10微米的特性長度。
基於前述種種考量，根據本發明實施例中的一電極中的最小尺度的矽或矽基底元件可在0.08到1μm的範圍中，較佳而言係為0.2μm至0.3μm或是於該範圍間。欲進一步確定較佳的表面面積對體積比，該第二最大尺度應至少為該最小尺度的兩倍大。
另一個考量為該等元件間的電性互連數量。對於如纖維或帶狀的延長元件來說，最大尺度越大，則獨立部件就更有可能彼此交叉，並於其間形成複數個連接。類似地，對於薄板或薄片狀部件來說，該等薄片或薄板越大，則它們越有可能彼此重疊。更進一步，一或兩個最大尺度越大，則在固定表面面積中係排列有更大量的矽，進一步係減少不可逆的電容。基於此等考量，該最大的或是最大的兩個尺度係選定為比該最小尺度大十倍，較佳而言為100或200倍大，或是於該範圍間。舉例來說，該全部長度或最大尺度的大小可為500μm。
當然將會可理解任何適宜的方法皆可被採用，以製造出上述的矽或矽基底元件。
舉例來說，藉由於適宜的矽或矽基底基板上形成柱狀物可製造纖維，並接著藉由適宜的方法將該等柱狀物拆卸以創造纖維。矽柱可如PCT/GB2007/000211中描述或是於美國申請案第10/049736號中的描述來製造。
矽帶狀物可經由顯影製程來製造，以此適切塑型的結構係製於一矽或矽基底基板上，並接著係藉由適宜的拆卸方法來自該基板將其拆卸。
薄板(或亦可為薄片)可利用矽薄膜沉積來製造，其係於少量黏性的基板上以導致矽薄板可拆卸。若該可拆卸的薄板分散了，則係形成薄片。
一旦該等矽或矽基底元件製造完成，則可作為鋰離子電化學電池的複合陽極中的主動材料。要製造複合陽極，該等元件可與聚偏二氟乙烯混合並與鑄造溶劑製成漿體，該溶劑係如N-甲基吡咯酮。此漿體可接著被施加或塗布於一金屬箔上或其他導體基板上，舉例來說可物理性地以一刀鋒或以其他適宜方法來產生一所需厚度的塗布膜，且接著係利用適宜的乾燥系統將該鑄造溶劑自該膜蒸發，其可應用被提高為50度C至140度C範圍中的溫度來將該複合膜單獨留下，或自該鑄造溶劑留下。該最終的複合膜具有多孔結構，其中矽或矽基底元件量一般係於百分之70與百分之95之間。該複合膜將會具有百分之10-30的孔洞體積百分比，較佳而言約為百分之20。
鋰離子電池單元的製造之後可以任何適宜的方法實行，舉例來說可接續圖1中所示的一般結構但具有矽或矽 基底主動陽極材料，而非石墨主動陽極材料。舉例來說，該矽元件基底複合陽極層係被該多孔間隔物18覆蓋，添加至最後結構的電解質係充滿全部的孔洞體積。將該電極置於適宜外箱中後，係完成電解質的添加，且可包含陽極的真空填充，以確保該孔洞體積係填滿該液態電解質。
本文中描述方法的一個特殊優點為可製造大薄板的矽基底陽極，並接著接續捲繞或停止，其係於鋰離子電池單元的石墨基底陽極的狀況，表示本文中描述的方法可對現存的製造能力作翻新。
當然將可了解，任何適宜的方法皆可被採用以達成上述的方法與設備。舉例來說，該元件的製造可包含矽製程工業中所應用的任何一種適合的方法。該陰極材料可為任何適合的材料，一般來說為鋰基底金屬氧化材料。該等元件可具有任何適合的尺度，舉例來說，也可為純矽或摻雜矽或其他矽基底材料，如矽鍺混合物或任何其他適宜的混合物。
上文描述僅經由舉例，而非用以限制該宣告主體物件的範疇，其係用以涵蓋任何上述實施例的修正、並置，或替換者，如熟習本技藝人士所認知。舉例來說，雖然以矽作為電極材料已特別描述於本文中，但也可應用其他矽基底材料來取代未摻雜的矽，如摻雜的矽，例如SiGe。
2‧‧‧可充電鋰離子電池單元
10‧‧‧銅電流收集器
12‧‧‧鋁電流收集器
14‧‧‧陽極層
16‧‧‧陰極層
18‧‧‧多孔間隔物
20‧‧‧間隔物或分隔物
圖1為可充電鋰離子電池單元的基本組成。
2‧‧‧可充電鋰離子電池單元
10‧‧‧銅電流收集器
12‧‧‧鋁電流收集器
14‧‧‧陽極層
16‧‧‧陰極層
18‧‧‧多孔間隔物
20‧‧‧間隔物或分隔物

Claims (14)

  1. 一種用於電化學電池的電極，其包含：複數個矽或矽基底元件，其具有在0.08μm至1.00μm範圍中的最小尺度；第一較大尺度，其至少為該最小尺度的兩倍大；及第二較大尺度，其中，該等元件包含互連部件並且係選自為帶狀、薄板或管狀。
  2. 如申請專利範圍第1項的電極，其中該矽或矽基底元件的第一與第二大尺度係具有類似大小。
  3. 如申請專利範圍第1項的電極，其中該最小尺度在0.2μm至0.3μm範圍中。
  4. 如申請專利範圍第1項的電極，其中該第一較大尺度為該最小尺度的5倍大。
  5. 如申請專利範圍第1項的電極，其中該第二較大尺度為該最小尺度的至少10倍大。
  6. 如申請專利範圍第5項的電極，其中該第二較大尺度為該最小尺度的100或200倍大。
  7. 一種複合電極，其包含如申請專利範圍第1至2項中任一項之矽或矽基底元件，其係作為其主動材料之一。
  8. 如申請專利範圍第7項的複合電極，其進一步包含一銅電流收集器。
  9. 如申請專利範圍第8項的複合電極，其中該電極為一陽極。
  10. 一種電化學電池，其包含如申請專利範圍第7至9項中任一項之電極。
  11. 如申請專利範圍第10項的電化學電池，其中該陰極包含鋰基底化合物作為其主動材料。
  12. 如申請專利範圍第11項的電化學電池，其中該陰極包含鋰基底金屬氧化物作為其主動材料。
  13. 一種裝置，其係由如申請專利範圍第10至12項中任一項之電化學電池所供電。
  14. 如申請專利範圍第12項的電化學電池，其中該陰極包含LiCoO2 。
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