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Operando Electrochemical Liquid Cell Scanning Transmission Electron Microscopy Investigation of the Growth and Evolution of the Mosaic Solid Electrolyte Interphase for Lithium-Ion Batteries
ACS Nano ( IF 15.8 ) Pub Date : 2023-10-13 , DOI: 10.1021/acsnano.3c06879
Walid Dachraoui 1, 2 , Robin Pauer 1 , Corsin Battaglia 2, 3, 4 , Rolf Erni 1, 5
Affiliation  

The solid electrolyte interphase (SEI) is a key component of a lithium-ion battery forming during the first few dischage/charge cycles at the interface between the anode and the electrolyte. The SEI passivates the anode–electrolyte interface by inhibiting further electrolyte decomposition, extending the battery’s cycle life. Insights into SEI growth and evolution in terms of structure and composition remain difficult to access. To unravel the formation of the SEI layer during the first cycles, operando electrochemical liquid cell scanning transmission electron microscopy (ec-LC-STEM) is employed to monitor in real time the nanoscale processes that occur at the anode–electrolyte interface in their native electrolyte environment. The results show that the formation of the SEI layer is not a one-step process but comprises multiple steps. The growth of the SEI is initiated at low potential during the first charge by decomposition of the electrolyte leading to the nucleation of inorganic nanoparticles. Thereafter, the growth continues during subsequent cycles by forming an island-like layer. Eventually, a dense layer is formed with a mosaic structure composed of larger inorganic patches embedded in a matrix of organic compounds. While the mosaic model for the structure of the SEI is generally accepted, our observations document in detail how the complex structure of the SEI is built up during discharge/charge cycling.

中文翻译:

Operando 电化学液体电池扫描透射电子显微镜研究锂离子电池马赛克固体电解质界面的生长和演化

固体电解质界面(SEI)是锂离子电池的关键组成部分,在前几次放电/充电循环期间在阳极和电解质之间的界面处形成。SEI 通过抑制电解质进一步分解来钝化阳极-电解质界面,从而延长电池的循环寿命。从结构和组成方面了解 SEI 的增长和演变仍然很难获得。为了揭示第一个循环中 SEI 层的形成过程,采用操作电化学液体电池扫描透射电子显微镜 (ec-LC-STEM) 实时监测原生电解质中阳极-电解质界面发生的纳米级过程环境。结果表明SEI层的形成不是一步过程而是包括多个步骤。SEI 的生长是在第一次充电期间通过电解质分解在低电势下引发的,从而导致无机纳米颗粒的成核。此后,在随后的循环中通过形成岛状层继续生长。最终,形成一个致密层,具有镶嵌结构,该结构由嵌入有机化合物基质中的较大无机斑块组成。虽然 SEI 结构的镶嵌模型已被普遍接受,但我们的观察详细记录了 SEI 的复杂结构是如何在放电/充电循环过程中建立的。
更新日期:2023-10-13
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