TW201607102A - 鋰硫電池 - Google Patents
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Abstract
本發明有關包含一陽極、一陰極以及一液態電解質之鋰硫電池;該陽極含有鋰金屬或鋰金屬合金,該陰極含有電活性硫材料及固體電導性材料的混合物,以及該液態電解質含有至少一鋰鹽及一包含二腈的溶劑。
Description
本發明係與一鋰硫電池相關。
傳統的鋰硫電池包括一陽極(正極)及一陰極(負極),陽極由鋰金屬或是鋰金屬合金形成,陰極由元素硫或是其它電活性硫材料形成。該硫或是其它含電活性硫材料可以與諸如碳之電性傳導材料混合,以改善其電導性。典型地,該碳及硫經研磨,而後與溶劑及黏合劑混合形成料漿。該料漿被施加於電流收集器上,而後被乾燥以移除溶劑。所獲得的結構經砑光以形成一複材結構,其經截切為所欲的形狀以形成陰極。將一隔離板放置於該陰極上,以及將一鋰陽極放於該隔離板上。將電解質引入該電池中以潤濕該陰極及隔離板。該電解質典型上包含溶於溶劑之電解鹽。
鋰硫電池為二次電池,且可藉由施加一外部電流至該電池而被再充電。此種型式之可再充電電池有廣泛的潛在用途。於發展鋰硫二次電池時的重要考量包括重量能量、週期壽命,以及電池組裝簡易性。
當鋰硫電池放電時,於陰極中的硫以二階段被還原。於第一階段,該電活性硫材料(例如:元素硫)被還原成為多硫化物類物質Sn 2-(n2)。此類物質一般溶於電解質中。於放電的第二階段中,該多硫化物類物質被還原為硫化鋰,Li2S,其係不溶解的。當電池被充電時,該二階段可逆地發生,該硫化鋰被氧化為多硫化鋰,以及再被氧化為鋰及硫。
除了作為一用於電解鹽的適合溶劑外,供使用於鋰硫電池的溶劑應該不與鋰金屬陽極反應,且可供作一於放電期間形成的多硫化物類物質的良好溶劑。因此,由於至少某個程度上由在鋰硫電池充電及放電過程間形成的中間物質被引入之多重維度,鋰硫電池的溶劑需求明顯地遠較鋰離子電池複雜。許多典型上被應用於鋰離子電池中溶劑,例如碳酸酯,不適合使用於鋰硫電池中,因為其會與在放電時形成的多硫化物反應,特別是在高硫負載的情況下。因此,於鋰硫電池中電解質溶劑的性能,無法由其作為一鋰離子電池的電解質溶劑的性能來作預測。
於描述本發明的特定實例前,要瞭解本揭示內容並不侷限於於此揭示之特定電池、方法或是材料。亦需瞭解於此所使用的術語僅係用以描述特定實例,而不是用作限制,因為本案所受保護的範圍係由申請專利範圍及其等效的範圍所限定。
圖1:使用鋰LiTDI(4,5-二氰-2-(三氟甲基)咪唑)以2-甲基戊二腈作電解質形成的鋰硫電池於各種溫度下的充電放電曲線。
圖2:使用環丁碸作為電解質形成之比較電池的比較充電放電曲線。
於描述與主張本發明之電池與方法的權利時,將使用以下的術語:單數形式的"一"以及"該"包括複數形,除非於上下文當中明白地另有它指。因此,述及"一陽極"包括述及一個或是一個以上如此的元件。
根據本發明之一態樣,提供一鋰硫電池,其包含:一陽極,其包含鋰金屬或是鋰金屬合金;一陰極,其包含電活性硫材料及固體電導性材料的混合物;以及一液態電解質,其包含至少一鋰鹽及含有二腈的溶劑。
於本發明之實施態樣中,已發現,藉由使用二腈作為電解質溶劑,能夠增加該鋰硫電池的重量能量。亦已發現,所形成的電解質使用二腈作為溶劑也可具有良好的黏性特徵。據此,此電解質可採用一習用且有效的方法被施加於陰極上,增進效能及便於電池組裝。於本發明之實施態樣中,亦已發現藉由在鋰硫電池中使用二腈作為溶劑,該鋰硫電池的週期壽命可被改良。
於本發明之實施態樣,已發現鋰硫電池的低溫性能可藉由使用二腈作為溶劑而改進。舉例言之,於某些實施態樣中,該電解質在低於0℃,例如,低於-10℃(如:直到-30℃)的溫度仍可維持液態。
該二腈具有式(I):
其中:n是2至10中之一整數,及於每個-CR1R2-鍵結,R1及R2係各自獨立地選自H、-OH、胺、醯胺、醚,及C1至C6烷基。
為免生疑慮,各個-CR1R2-鍵結可相同或是相異。於一實施態樣中,於該二腈中之一-CR1R2-鍵結不同於其它的-CR1R2-鍵結。該不同於其它-CR1R2-鍵結之-CR1R2-鍵結可存在於鄰近CN基處。
於此R1及/或R2為胺,該胺可具有式-NRaRb,於此各個Ra及Rb係獨立地為H或是烴基。適合的烴基包括烷基,例如C1至C4烷基(如:甲基、乙基、丙基或丁基)。舉例言之,-NRaRb可為-NH2或是-N(CH3)2。該胺可為一級、二級或是三級胺。
於此R1及/或R2為醯胺,該醯胺可為-NRaC(O)Rb,於此各個Ra及Rb可各自獨立地為H或是烴基。適合的烴基包
括烷基,例如C1至C4烷基(如:甲基、乙基、丙基或丁基)。舉例言之,-NRaC(O)Rb可為-NHC(O)CH3。
於此R1及/或R2為醚,該醚可具有式-ORc,於此Rc為烴基。適合的烴基包括烷基,例如C1至C4烷基(如:甲基、乙基、丙基或丁基)。舉例言之,-ORc基可為-OCH3。
於此R1及/或R2可為烷基,該烷基可為C1至C6烷基,如:甲基、乙基、丙基、i-丙基、n-丁基、i-丁基、t-丁基、戊基或己基。
於一實施態樣中,該式(I)之二腈包括有至少2個,例如2至4個式-CH2-之-CR1R2-鍵結。可選擇地,該式(I)之二腈可包括一或二個式-CHR2-之-CR1R2-鍵結。該-CHR2-鍵結可鄰近-CN基。
於一實施態樣中,該二腈具有式(II):
其中:p是0或1,q是1至9中之一整數,r是0或1,以及R3、R4、R5及R6係各自獨立地選自H及C1至C6烷基(如:甲基、乙基、丙基、i-丙基、n-丁基、i-丁基、t-丁基、戊基或己基,較佳為甲基)。
較佳地,至少R3及R4之一為H,以及至少R5及R6之一為H。較佳地,至少R3、R4、R5及R6之一為C1至C6烷基。於一實施態樣,R3為H;R5為H;以及至少R4及R6之一為C1至C6烷基。舉例言之,於一實施態樣中,R3為H;R5為H;R4為H以及R6為C1至C6烷基。
於一實施態樣中,p為0及r為1。於一實施態樣中,,q為2。舉例言之,P可為0、r可為1以及q可為2。
適當二腈之實例包括2-甲基戊二腈、琥珀腈,以及己二腈。
如先前所述,該電解質亦可包含一鋰鹽。適合的鋰鹽包括六氟磷酸鋰(LiPF6)、六氟砷酸鋰(LiAsF6)、過氯酸鋰(LiClO4)、三氟甲烷磺醯亞胺鋰(LiN(CF3SO2)2)、硼氟酸鋰(LiBF4)、三氟甲烷磺酸鋰(CF3SO3Li),以及雙草酸硼酸鋰(LiB(C2O4)2)。較佳地,該鋰鹽為三氟甲烷磺醯亞胺鋰(LiN(CF3SO2)2)。
於電解質中鋰鹽的濃度較佳為0.1至5M、更佳地為0.2至3M,舉例言之,0.4至2M(如:0.5至1M)。
如先前所論及者,本發明之鋰硫電池包括一陽極、一陰極、一電解質,以及可選擇地一多孔隔離板。後者可置於該陽極與陰極之間。該陽極由鋰金屬或是鋰金屬合金所形成。較佳地,該陽極為一金屬箔電極,諸如一鋰箔電極。該鋰箔是由鋰金屬與鋰金屬合金形成。
該電池的陰極包含一電活性硫材料與電導性材料的混合物。該混合物形成一電活性層,其可經安置與一
電流收集器相接觸。
該電活性硫材料可包含元素硫、以硫為主之有機化合物、以硫為主之無機化合物,以及含硫聚合物。較佳地,使用元素硫。
該固體電導性材料可為任何適合的傳導材料。較佳地,該固體電導性材料可由碳形成。實例包括碳黑、碳纖維、單層石墨及碳奈米管。其餘適合的材料包括金屬(如:小片、銼屑及粉末)以及傳導聚合物。較佳地,使用碳黑。
電活性硫材料與電導性材料之混合物,可採用於一溶劑(如:水或是有機溶劑)中之料漿的形式,被施加於電流收集器上。接下來將該溶劑移除,以及令所獲得的結構被砑光以形成一複材結構,其可被截切成所欲形狀以形成一陰極。一隔離板可被安置於該陰極上,以及一鋰陽極可被安置於該隔離板上。接下來電解質被併入該經組裝的電池中以潤濕該陰極與隔離板。
可替代地,在陰極形成之後,該電解質可被塗覆於該陰極上。接下來將該隔離板安置於該經塗覆的陰極上,以及將陽極安置於該隔離板上。
如先前所述,使用二腈作為溶劑所形成的電解質亦可具有良好的黏性特徵。因此,該電解質可採用一習用且有效的方法被施加於陰極上,增進效能及便於電池組裝。於一較佳實施態樣中,藉由於陰極上塗覆電解質令電解質被併入電池總成,於該經塗覆之陰極上安置隔離板,以及於該隔離板上安置陽極。該塗覆可使用任何適當的方法實
行,例如,在該活性硫材料上藉由噴灑、擠塑、真空充填、傾注及/或塗布電解質。於該電解質被併入於電池總成後,該電池可被封緘,於例如一封圍中。該封圍可為不透水及/或不透氣的。適合的封圍包括一小袋。
於此隔離板被採用,該隔離板可包含任何容許離子於電池之電極間移動的適當的多孔材質。該隔離板應被放置於該等電極間以避免電極間直接接觸。該材質的多孔性至少應為30%,較佳為至少50%,例如,高於60%。較佳地,該隔離板的多孔性為40-60%,更佳為45-55%,例如50%。適合的隔離板包含有由聚合性材料形成的孔目。適合的聚合物包括聚丙烯、尼龍及聚乙烯。非織造的聚丙烯特別適合。使用多層的隔離板亦可行。
較佳地,該隔離板係擇自非織造聚丙烯及聚乙烯。
較佳地,該隔離板的可滲透性少於300 Gurley,較佳少於250 Gurley,例如200 Gurley。
本發明之鋰硫電池為二次電池。當該鋰硫電池放電時,該陰極中的硫以二階段被還原。於第一階段,該電活性硫材料(例如:元素硫)被還原成為多硫化物類物質Sn 2-(n2)。此類物質一般溶於電解質中。於放電的第二階段中,該多硫化物類物質被還原為硫化鋰,Li2S,其典型上沉積於該陽極的表面上。
當電池被充電時,該二階段機制可逆地發生,該硫化鋰被氧化為多硫化鋰,以及再被氧化為鋰及硫。因此,
該電池之電解質可包含溶於二腈中的多硫化物類物質。
實施例1
藉由將雙三氟甲烷磺醯亞胺鋰(LiTFSi)以0.5M的濃度溶入下表中所列溶劑製備所有的電解質。電解質接下來於30℃攪拌歷時1小時或直至完全溶解。
接下來於乾燥室條件(露點<-50℃)下,電解質被併入組成的電池中。陰極材料由硫、碳黑及聚氧化乙烯(PEO)以70:10:20(w/w)之比例分別構成。該陰極材料典型以1.9-2.0mAh/cm2之表面容量被鑄於經鋁塗覆之碳上。電池藉由以電解質(3.5μL/mAh/cm2)潤濕陰極來組成,其與隔離板(Celgard 3501)及厚100μm之鋰箔陽極順序堆疊。
在1.5-2.45V之電壓範圍間,於30℃,使用瑪科隆多渠道周期計(Maccor multi-channel cycler)以定電流放電之模式評估該等電池的放電-充電性能。該等電池分別於0.2C及0.1C之電流密度放電及充電。
下表顯示各個電池的重量能量密度。其與一使用於環丁碸中0.5M雙三氟甲烷磺醯亞胺鋰(LiTFSI)所形成的參考電池比較。可由該表中發現,相較於參考電池以及使用單腈作為電解質溶劑的電池,使用二腈作為電解質溶劑的顯示了明顯改進的重量能量密度。
實施例2
使用鋰LiTDI(4,5-二氰-2-(三氟甲基)咪唑)溶於2-甲基戊二腈(2-MGN)中作為電解質形成的鋰硫電池在-10至30℃的溫度範圍中循環。於圖1顯示在各種溫度下的充電放電曲線。使用環丁碸作為電解質溶劑形成一比較電池。於圖2顯示比較充電放電曲線。由圖中可看出,使用2-MGN作為電解質溶劑於低溫下具有優異的性能。
Claims (13)
- 一種鋰硫電池,其包含:一陽極,其含有鋰金屬或是鋰金屬合金;一陰極,其含有電活性硫材料及固體電導性材料之混合物;以及一液態電解質,其含有至少一鋰鹽及一含有二腈的溶劑。
- 如請求項1之電池,其中該二腈具有式(I):
- 如請求項2之電池,其中該二腈具有式(II):
- 如請求項3之電池,其中R3及R4之至少一者為H,以及R5及R6之至少一者為H。
- 如請求項3或4之電池,其中R3、R4、R5及R6之至少一者為C1至C6烷基。
- 如請求項3至5中任一項之電池,其中p為0以及r為1。
- 如請求項6之電池,其中q為2。
- 如請求項6或7之電池,其中R5及R6之至少一者為H,而另一者為C1至C6烷基。
- 如請求項2至8中任一項之電池,其中該C1至C6烷基為甲基。
- 如請求項1之電池,其中該二腈係選自2-甲基戊二腈、琥珀腈,以及己二腈。
- 如請求項1至10中任一項之電池,其中該電解質進一步包含溶於二腈當中的多硫化鋰。
- 如請求項1至11中任一項之電池,其中該電活性硫材料包含元素態硫。
- 如請求項1至12中任一項之電池,其中該固體電導性材料包含碳。
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-
2015
- 2015-05-21 CN CN201580029063.2A patent/CN106537660B/zh active Active
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ES2700576T3 (es) | 2019-02-18 |
JP6662522B2 (ja) | 2020-03-11 |
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PL3149792T3 (pl) | 2019-04-30 |
KR20170012338A (ko) | 2017-02-02 |
EP3149792A1 (en) | 2017-04-05 |
CN106537660A (zh) | 2017-03-22 |
KR102445459B1 (ko) | 2022-09-20 |
CA2950513A1 (en) | 2015-12-03 |
CN106537660B (zh) | 2020-08-14 |
WO2015181527A1 (en) | 2015-12-03 |
CA2950513C (en) | 2023-04-04 |
HUE042287T2 (hu) | 2019-06-28 |
TWI670881B (zh) | 2019-09-01 |
US10811728B2 (en) | 2020-10-20 |
US20170200977A1 (en) | 2017-07-13 |
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