Slurry-Fabricable Li+-Conductive Polymeric Binders for Practical All-Solid-State Lithium-Ion Batteries Enabled by Solvate Ionic Liquids
Slurry-Fabricable Li+-Conductive Polymeric Binders for Practical All-Solid-State Lithium-Ion Batteries Enabled by Solvate Ionic Liquids
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DOI：
10.1002/aenm.201802927
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发表时间：
2019-04-25
影响因子：
27.8
通讯作者：
Jung, Yoon Seok
中科院分区：
文献类型：
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作者：
Oh, Doe Yang;Nam, Young Jin;Jung, Yoon Seok
为了大规模生产采用高 Li+ 导电性和可机械烧结的硫化物固体电解质 (SE) 的全固态锂离子电池 (ASLB)，湿法浆料工艺势在必行。不幸的是，硫化物SE的化学稳定性差，严重限制了溶剂和聚合物粘合剂的可用候选者。此外，粘合剂会中断界面处的Li+离子接触，导致电化学性能低于标准。在这项工作中，报告了一种新的可扩展浆料制造方案，用于由 Li+ 导电聚合物粘合剂制成的片状 ASLB 电极。在浆料中使用中等极性溶剂（例如二溴甲烷）可以将 Li6PS5Cl 和溶剂化离子液体基聚合物粘合剂（NBR-Li(G3) TFSI、NBR：丁腈橡胶、G3：三甘醇二甲醚、LiTFSI：双（三氟甲磺酰基）酰亚胺锂）一起容纳，而不会发生不良副反应或相分离。采用NBR-Li(G3) TFSI的LiNi0.6Co0.2Mn0.2O2和Li4Ti5O12电极在30℃下分别表现出174和160 mAh g(-1)的高容量，远远优于使用传统NBR的电极（144和76 mAh g(-1)）。此外，LiNi0.7Co0.15Mn0.15O2电极具有7.4 mA h cm(-2)的高面积容量和45 mg cm(-2)的超高质量负载。电化学和 7Li 核磁共振测量的补充分析证明了 NBR-Li(G3) TFSI 铺就的界面处促进了 Li+-离子接触。
For mass production of all-solid-state lithium-ion batteries (ASLBs) employing highly Li+ conductive and mechanically sinterable sulfide solid electrolytes (SEs), the wet-slurry process is imperative. Unfortunately, the poor chemical stability of sulfide SEs severely restrict available candidates for solvents and in turn polymeric binders. Moreover, the binders interrupt Li+-ionic contacts at interfaces, resulting in the below par electrochemical performance. In this work, a new scalable slurry fabrication protocol for sheet-type ASLB electrodes made of Li+-conductive polymeric binders is reported. The use of intermediatepolarity solvent (e.g., dibromomethane) for the slurry allows for accommodating Li6PS5Cl and solvate-ionic-liquid-based polymeric binders (NBR-Li(G3) TFSI, NBR: nitrile-butadiene rubber, G3: triethylene glycol dimethyl ether, LiTFSI: lithium bis(trifluoromethanesulfonyl) imide) together without suffering from undesirable side reactions or phase separation. The LiNi0.6Co0.2Mn0.2O2 and Li4Ti5O12 electrodes employing NBR-Li(G3) TFSI show high capacities of 174 and 160 mA h g(-1) at 30 degrees C, respectively, which are far superior to those using conventional NBR (144 and 76 mA h g(-1)). Moreover, high areal capacity of 7.4 mA h cm(-2) is highlighted for the LiNi0.7Co0.15Mn0.15O2 electrodes with ultrahigh mass loading of 45 mg cm(-2). The facilitated Li+-ionic contacts at interfaces paved by NBR-Li(G3) TFSI are evidenced by the complementary analysis from electrochemical and 7Li nuclear magnetic resonance measurements.