全固態電池現今是個極具發展性及有趣性的研究領域，能避免大量液態電解液造成潛在的爆炸、漏液危險，且能直接使用鋰金屬當作負極，透過減少體積來提高能量密度，而電解質中又以固態硫化物電解質最為突出，因其擁有最高的導離子度與熱穩定性。但組裝出硫化物全固態電池需要在惰性氣氛下進行，並且要克服介面接觸不良以及副反應問題。
本研究分為兩個部分，一為全固態電池的組裝，從錠狀電池到膜狀電池，並探討正極、負極、固態電解質的各個參數的影響。使用LNO@NCM811高鎳三元材料當作正極，Li6PS5Cl作為固態電解質，鋰與銦金屬作為負極，1 wt %的添加碳，第二部分為軟包電池組裝，成功組裝出3x3 cm2大小的NMC811||LPSC||In 軟包全固態電池，充電區間2 V~3.9 V、0.02 C，於室溫(25℃)下施予17.5 MPa之外壓，首圈電容高達153.44 mAh/g (2.056 mAh/cm2)，經15圈充放電後還有71.6 %以上的維持率。
另一部分為混和型固態電池，電池中同時包含了液態電解液及固態電解質，而使用的正極極片為目前商用製程樣品，而非複合正極，正極中沒有添加固態電解質。液態電解液添加於正極側，扮演著鋰離子通道的角色，這有兩項優點，一是透過使用一般正極極片省去了處理複合正極對濕氣敏感性的問題，二是透過液態電解液來改善介面接觸不良的問題。本文引入了溶劑化的概念，以溶劑化結構來降低溶劑對硫化物的反應性，使用LiTFSI溶於FEC/TTE/EMC，再依據拉曼光譜鑑定液態電解液與固態電解質之相容性，確保液固兩者能穩定並存於電池中。最後亦將此技術應用於軟包電池中，添加少量電解液 (1.1~1.3 μl/ mAh) 於電池中，開發出NMC811||Liquid electrolyte||LPSC||SUS軟包無陽極準固態電池，充電區間2.5 V~4.3 V，僅施予1.5 MPa之外壓，使用1.5 M濃度的電解液，第二圈電容154.76 mAh/g，總電容高達27.7 mAh，但其壽命是個問題，第十圈時維持率約剩下50 %，還有很大的優化空間。但此項技術是一大突破且已申請專利，使硫化物固態電池離商業化更進了一步，最終建立好測試方法與平台，成功組裝出本實驗第一顆固態軟包電池。

Nowadays, all solid-state lithium battery (ASSLB) has been a promising and attractive research topic. This kind of battery avoids flammability and leakage of the liquid electrolyte. Besides, it can use lithium as an anode to increase energy density by decreasing the anode volume. Among various solid electrolytes, sulfide-type electrolyte stands out above the rest category of solid electrolytes as it has the highest ionic conductivity and best thermal stability. However, it’s not effortless to practically fabricate ASSLB considering some problems have to be overcome, such as the poor interface contact issue and side reactions between solid electrolytes and electrodes.
This research is divided into two parts, fabrication, and analysis of each ASSLBs and hybrid solid-state batteries. For the first part, we integrate the parameters of cathodes, anodes, and solid electrolytes for proceeding from pellet to film-type cell. The materials used for cells are LNO@NCM811 as cathode, Li6PS5Cl as solid electrolyte, lithium and indium as an anode, and 1 wt. % of additive carbon. With these prerequisites, we fabricate the NMC811||LPSC||In ASSLB pouch cell with the size of 3x3 cm2 which means we successfully scale up the manufacture from laboratory to pilot-scale. The electrochemical performance is displayed with the charging conditions ranging from 2 to 3.9 V and applied pressure of 17.5 MPa. The capacity of the first cycle is up to 153.44 mAh/g (2.056 mAh/cm2), and it still has 71.6 % capacity retention after 15 cycles.
Another part is hybrid solid electrolyte batteries which contain both liquid and solid electrolyte. We use commercial cathode instead of a composite one, thus there is no solid electrolyte. Besides that, liquid electrolyte added on the side of the cathode is taken as lithium transport pathways. There are two merits for this case, no moisture sensibility for common electrode and better interface contact since liquid takes part in it.
Here we introduce the concept of solvation, which is the attraction of the lithium salt for the polar electrolyte. Likewise, we use LiTFSI solvated in FEC/TTE/EMC. The compatibility of liquid and solid is characterized by Raman spectroscopy to see if the two phases can coexist in the battery. Subsequently, we introduce this technique from coin cell to pouch cell. By adding a small quantity of liquid electrolyte (1.1~1.3 μl/ mAh) to the cell, we develop an anode free hybrid solid-state battery, NMC811||Liquid electrolyte||LPSC||SUS. With the condition of charging range from 2.5 to 4.3V, applied pressure of only 1.5 MPa, and 1.5M electrolyte, the capacity of second cycle is 154.76 mAh/g and the total capacity reaches 27.7 mAh. However, the cycle life is a big issue as the retention is only 50 % in the 10th cycle. For that matter, there is still much room for improvement. Nevertheless, we have already established a good method for electrochemical measurement and successfully assembled the solid-state pouch cell. This technique is a significant milestone for ASSLB to be commercialized and has been patented.

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