Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 62, Issue 1, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202215414
Keywords
Energy Storage; Ferromagnetic Element; Insoluble Li2S2-Li2S Reduction; Lithium-Sulfur Battery; Polar Single-Atom Catalysts
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Funding
- National Natural Science Foundation of China [52273269, 52161145402, 52173133]
- Sichuan Science and Technology Program [2021YFH0180]
- 1.3.5 Project for Disciplines of Excellence, West China Hospital, Sichuan University [ZYJC21047]
- innovation project of Med-X Center for Materials, Sichuan University [MCM202102]
- State Key Laboratory of Polymer Materials Engineering [sklpme2022-3-07, sklpme2021-4-02]
- Projekt DEAL
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This study reveals the origin of Li2S2-Li2S reduction catalysis in single-atom materials based on ferromagnetic elements, attributing it to the spin density and magnetic moments. Experimental and theoretical studies show that Fe-N-4-based cathodes exhibit the fastest deposition kinetics of Li2S and the lowest thermodynamic energy barriers. Accelerated Li2S2-Li2S reduction catalysis enabled via spin polarization provides practical opportunities for long-life batteries.
Accelerating insoluble Li2S2-Li2S reduction catalysis to mitigate the shuttle effect has emerged as an innovative paradigm for high-efficient lithium-sulfur battery cathodes, such as single-atom catalysts by offering high-density active sites to realize in situ reaction with solid Li2S2. However, the profound origin of diverse single-atom species on solid-solid sulfur reduction catalysis and modulation principles remains ambiguous. Here we disclose the fundamental origin of Li2S2-Li2S reduction catalysis in ferromagnetic elements-based single-atom materials to be from their spin density and magnetic moments. The experimental and theoretical studies disclose that the Fe-N-4-based cathodes exhibit the fastest deposition kinetics of Li2S (226 mAh g(-1)) and the lowest thermodynamic energy barriers (0.56 eV). We believe that the accelerated Li2S2-Li2S reduction catalysis enabled via spin polarization of ferromagnetic atoms provides practical opportunities towards long-life batteries.
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