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Unveiling the autocatalytic growth of Li2S crystals at the solid-liquid interface in lithium-sulfur batteries

Zhen Wu, Mingliang Liu, Wenfeng He, Tong Guo, Wei Tong, Erjun Kan, Xiaoping Ouyang (), Fen Qiao, Junfeng Wang, Xueliang Sun, Xin Wang, Junwu Zhu (), Ali Coskun () and Yongsheng Fu ()
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Zhen Wu: Nanjing University of Science and Technology
Mingliang Liu: Nanjing University of Science and Technology
Wenfeng He: Nanjing University of Science and Technology
Tong Guo: Nanjing University of Science and Technology
Wei Tong: Nanjing University of Science and Technology
Erjun Kan: Nanjing University of Science and Technology
Xiaoping Ouyang: Xiangtan University
Fen Qiao: Jiangsu University
Junfeng Wang: Jiangsu University
Xueliang Sun: University of Western Ontario
Xin Wang: Nanjing University of Science and Technology
Junwu Zhu: Nanjing University of Science and Technology
Ali Coskun: University of Fribourg
Yongsheng Fu: Nanjing University of Science and Technology

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Electrocatalysts are extensively employed to suppress the shuttling effect in lithium-sulfur (Li-S) batteries. However, it remains challenging to probe the sulfur redox reactions and mechanism at the electrocatalyst/LiPS interface after the active sites are covered by the solid discharge products Li2S/Li2S2. Here, we demonstrate the intrinsic autocatalytic activity of the Li2S (100) plane towards lithium polysulfides on single-atom nickel (SANi) electrocatalysts. Guided by theoretical models and experimental data, it is concluded that LiPS dissociates into Li2S2 and short-chain LiPS on the Li2S (100) plane. Subsequently, Li2S2 undergoes further lithiation to Li2S on the Li2S (100) surface, generating a new Li2S (100) layer, thus enabling the autocatalytic formation of a new Li2S (100) surface. Benefiting from the autocatalytic growth of Li2S, the concentration of LiPS in the electrolyte remains at a lower level, enabling Li-S batteries under high loading and low electrolyte conditions to exhibit superior electrochemical performance.

Date: 2024
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DOI: 10.1038/s41467-024-53797-y

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