Synchronously Consolidating Li, Se, S, and C for Robust Li-SeS Batteries

Mengmeng Qian, Feng Wu*, Junfan Zhang, Yun Li, Chongteng Wu, Duanyun Cao, Jing Wang, Tinglu Song, Longlong Fan, Yifei Yuan, Jia Qi Huang, Guoqiang Tan*

*此作品的通讯作者

科研成果: 期刊稿件文章同行评审

摘要

S-redox involving solvated polysulfides is accompanied by volumetric change and structural decay of the S-based cathodes. Here, we propose a synchronous construction strategy for consolidating Li, Se, S, and C elements within a composite cathode via a paradigm reaction of 8Li+2Se+CS2 = 2Li4SeS+C. The obtained composite features crystalline Li4SeS encapsulated in a carbon nanocage (Li4SeS@C), exhibiting ultrahigh electrical conductivity, ultralow activation barrier, and excellent structural integrity, accordingly enabling large specific capacity (615 mAh g-1) and high capacity retention (87.3% after 350 cycles) at 10 A g-1. TOF-SIMS demonstrates its superior volumetric efficiency to a similar derivative SeS@C (2Se+CS2 = 2SeS+C), and DFT reveals its lower activation barrier than Li2S@C and Li2Se@C. This consolidation design significantly improves the electrochemical performance of S-based cathodes, and the paradigm reaction guarantees structural diversity and flexibility. Moreover, employing a synchronous construction mechanism to maximize the synergistic effect between element consolidation and carbon encapsulation opens up a new approach for developing robust S or chalcogenide cathodes.

源语言英语
期刊Nano Letters
DOI
出版状态已接受/待刊 - 2024

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