Tracking Passivation and Cation Flux at Incipient Solid‐Electrolyte Interphases on Multi‐Layer Graphene using High Resolution Scanning Electrochemical Microscopy
Tracking Passivation and Cation Flux at Incipient Solid‐Electrolyte Interphases on Multi‐Layer Graphene using High Resolution Scanning Electrochemical Microscopy
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DOI：
10.1002/celc.202101445
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发表时间：
2022-03
期刊：
影响因子：
4
通讯作者：
Yunxiong Zeng;Z. Gossage;Dipobrato Sarbapalli;Jingshu Hui;J. Rodríguez‐López
中科院分区：
文献类型：
--
作者：
Yunxiong Zeng;Z. Gossage;Dipobrato Sarbapalli;Jingshu Hui;J. Rodríguez‐López
固体电解质界面 (SEI) 是一种动态的电子绝缘膜，形成于锂离子电池 (LIB) 的负极上，使离子能够进出界面，同时防止电解质击穿。然而，对于新兴电池概念中在 Na+ 和 K+ 电解质上形成的 LIB SEI 的比较了解有限。我们使用扫描电化学显微镜 (SECM) 对多层石墨烯上形成的 Li+、K+ 和 Na+ 电解质中的初始 SEI 进行原位界面分析。使用 300 nm SECM 探针和离子敏感测量的反馈图像表明，与 Na+ 和 K+-SEI 相比，Li+-SEI 具有优异的钝化和最高的阳离子通量。非原位 X 射线光电子能谱表明，仅 Li+ 和 Na+-SEI 形成了显着的氟化物，这使得与原位 SECM 测量相关。虽然 SEI 化学仍然很复杂，但这些电分析方法揭示了化学变量与储能材料界面特性之间的联系。
The solid electrolyte interphase (SEI) is a dynamic, electronically insulating film that forms on the negative electrode of Li+batteries (LIBs) and enables ion movement to/from the interface while preventing electrolyte breakdown. However, there is limited comparative understanding of LIB SEIs with respect to those formed on Na+and K+electrolytes for emerging battery concepts. We used scanning electrochemical microscopy (SECM) for the in situ interfacial analysis of incipient SEIs in Li+, K+and Na+electrolytes formed on multi‐layer graphene. Feedback images using 300 nm SECM probes and ion‐sensitive measurements indicated a superior passivation and highest cation flux for a Li+‐SEI in contrast to Na+and K+‐SEIs. Ex situ X‐ray photoelectron spectroscopy indicated significant fluoride formation for only Li+and Na+‐SEIs, enabling correlation to in situ SECM measurements. While SEI chemistry remains complex, these electroanalytical methods reveal links between chemical variables and the interfacial properties of materials for energy storage.