Visualizing interfacial collective reaction behaviour of Li–S batteries

Shiyuan Zhou, Jie Shi, Sangui Liu, Gen Li, Fei Pei, Youhu Chen, Junxian Deng, Qizheng Zheng, Jiayi Li, Chen Zhao, Inhui Hwang, Cheng-Jun Sun, Yuzi Liu, Yu Deng, Ling Huang, Yu Qiao, Gui-Liang Xu (), Jian-Feng Chen, Khalil Amine (), Shi-Gang Sun and Hong-Gang Liao ()
Additional contact information
Shiyuan Zhou: Xiamen University
Jie Shi: Beijing University of Chemical Technology
Sangui Liu: Xiamen University
Gen Li: Xiamen University
Fei Pei: Xiamen University
Youhu Chen: Xiamen University
Junxian Deng: Xiamen University
Qizheng Zheng: Xiamen University
Jiayi Li: Nanjing University
Chen Zhao: Argonne National Laboratory
Inhui Hwang: Argonne National Laboratory
Cheng-Jun Sun: Argonne National Laboratory
Yuzi Liu: Argonne National Laboratory
Yu Deng: Nanjing University
Ling Huang: Xiamen University
Yu Qiao: Xiamen University
Gui-Liang Xu: Argonne National Laboratory
Jian-Feng Chen: Beijing University of Chemical Technology
Khalil Amine: Argonne National Laboratory
Shi-Gang Sun: Xiamen University
Hong-Gang Liao: Xiamen University

Nature, 2023, vol. 621, issue 7977, 75-81

Abstract: Abstract Benefiting from high energy density (2,600 Wh kg−1) and low cost, lithium–sulfur (Li–S) batteries are considered promising candidates for advanced energy-storage systems1–4. Despite tremendous efforts in suppressing the long-standing shuttle effect of lithium polysulfides5–7, understanding of the interfacial reactions of lithium polysulfides at the nanoscale remains elusive. This is mainly because of the limitations of in situ characterization tools in tracing the liquid–solid conversion of unstable lithium polysulfides at high temporal–spatial resolution8–10. There is an urgent need to understand the coupled phenomena inside Li–S batteries, specifically, the dynamic distribution, aggregation, deposition and dissolution of lithium polysulfides. Here, by using in situ liquid-cell electrochemical transmission electron microscopy, we directly visualized the transformation of lithium polysulfides over electrode surfaces at the atomic scale. Notably, an unexpected gathering-induced collective charge transfer of lithium polysulfides was captured on the nanocluster active-centre-immobilized surface. It further induced an instantaneous deposition of nonequilibrium Li2S nanocrystals from the dense liquid phase of lithium polysulfides. Without mediation of active centres, the reactions followed a classical single-molecule pathway, lithium polysulfides transforming into Li2S2 and Li2S step by step. Molecular dynamics simulations indicated that the long-range electrostatic interaction between active centres and lithium polysulfides promoted the formation of a dense phase consisting of Li+ and Sn2− (2

Date: 2023
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DOI: 10.1038/s41586-023-06326-8

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