Identifying the Critical Anion–Cation Coordination to Regulate the Electric Double Layer for an Efficient Lithium‐Metal Anode Interface,Angewandte Chemie International Edition

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Identifying the Critical Anion–Cation Coordination to Regulate the Electric Double Layer for an Efficient Lithium‐Metal Anode Interface
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-12-15 , DOI: 10.1002/anie.202013271
Rui Xu ₁ , Xin Shen ₂ , Xia-Xia Ma ₃ , Chong Yan ₁ , Xue-Qiang Zhang ₂ , Xiang Chen ₂ , Jun-Fan Ding ₁ , Jia-Qi Huang ₄

Affiliation

The persistent efforts to reveal the formation and evolution mechanisms of solid electrolyte interphase (SEI) are of fundamental significance for the rational regulation. In this work, through combined theoretical and experimental model investigations, we elucidate that the electric double layer (EDL) chemistry at the electrode/electrolyte interface beyond the thermodynamic stability of electrolyte components predominately controls the competitive reduction reactions during SEI construction on Li metal anode. Specifically, the negatively‐charged surface of Li metal will prompt substantial cation enrichment and anion deficiency within the EDL. Necessarily, only the species participating in the solvation shell of cations could be electrostatically accumulated in proximity of Li metal surface and thereafter be preferentially reduced during sustained dynamic cycling. Incorporating multi‐valent cation additives to more effectively drag the favorable anionic SEI enablers into EDL is validated as a promising strategy to upgrade the Li protection performance. The conclusions drawn herein afford deeper understandings to bridge the EDL principle, cation solvation, and SEI formation, shedding fresh light on the targeted regulation of reactive alkali metal interfaces.

中文翻译：

确定关键的阴离子-阳离子配位以调节双电层，实现高效的锂金属阳极界面

不断努力揭示固体电解质相（SEI）的形成和演化机理对于合理调节具有根本意义。在这项工作中，通过理论和实验模型相结合的研究，我们阐明了电极/电解质界面处的双电层（EDL）化学物质超出了电解质组分的热力学稳定性，主要控制了在Li金属阳极上进行SEI构造过程中的竞争性还原反应。特别是，锂金属带负电的表面将促使EDL中出现大量阳离子富集和阴离子不足。一定，只有参与阳离子溶剂化壳层的物质才能在锂金属表面附近静电积累，然后在持续动态循环中被优先还原。经验证，掺入多价阳离子添加剂可更有效地将有利的阴离子SEI促成剂引入EDL中，这是提高Li保护性能的有前途的策略。本文得出的结论为桥接EDL原理，阳离子溶剂化和SEI的形成提供了更深入的理解，为反应性碱金属界面的目标调节提供了新的思路。

更新日期：2021-02-12

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