Chemo-electrochemical Evolution of Cathode–Solid Electrolyte Interface in All-Solid-State Batteries,ACS Energy Letters

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Chemo-electrochemical Evolution of Cathode–Solid Electrolyte Interface in All-Solid-State Batteries
ACS Energy Letters ( IF 19.3 ) Pub Date : 2024-09-05 , DOI: 10.1021/acsenergylett.4c02062
Patrick J. Kwon _{1,

2} , Carlos Juarez-Yescas _{1,

2,

3} , Hyewon Jeong _{1,

2} , Saeed Moradi _{1,

2,

4} , Elizabeth Gao ₅ , Debbie Lawrence ₅ , Beniamin Zahiri _{1,

2} , Paul V. Braun _{1,

2,

3,

4,

6}

Affiliation

The stability of the interface between the cathode and the solid electrolyte (SE) has been found to be a key determinant of solid-state battery (SSB) performance. While interfacial failure from electrochemical cycling has been studied, temperature effects on the chemical and electrochemical evolution of interface properties are not well-understood. We utilize a dense additive-free LiCoO₂ cathode, which provides controlled morphology and crystallography, and well-known high voltage halide SEs (Li₃InCl₆ and Li₃YCl₆) to eliminate the need for cathode coating to explore the nature of interface deterioration induced by operating at up to 100 °C. By promoting temperature-induced accelerated interfacial failure, we show that at elevated temperatures (>60 °C) and higher states of charge, a significant chemo-electrochemical contribution to interfacial resistance results in rapid cell performance degradation. Our findings show that beyond the well sought-after SE electrochemical voltage stability, the atomic-scale restructuring of the cathode surface interfaced with the SE must be considered when designing stable interfaces.

中文翻译：

全固态电池中阴极-固体电解质界面的化学电化学演变

阴极和固体电解质（SE）之间界面的稳定性已被发现是固态电池（SSB）性能的关键决定因素。虽然已经研究了电化学循环引起的界面失效，但温度对界面特性的化学和电化学演变的影响尚不清楚。我们利用致密的无添加剂 LiCoO₂ 阴极，提供受控的形态和晶体学，以及众所周知的高压卤化物 SE（Li₃InCl₆ 和 Li₃YCl₆），无需阴极涂层即可探索在高达 100 °C 下操作引起的界面劣化的性质。通过促进温度诱导的加速界面失效，我们表明在高温（>60 °C）和较高的电荷状态下，对界面电阻的显着化学电化学贡献导致电池性能快速下降。我们的研究结果表明，除了广受欢迎的 SE 电化学电压稳定性之外，在设计稳定的界面时，还必须考虑与 SE 界面的阴极表面的原子级重构。

更新日期：2024-09-05

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