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Catalytic role of in-situ formed C-N species for enhanced Li2CO3 decomposition

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  • Fangli Zhang

    (Central South University
    The University of Adelaide
    University of Wollongong, Faculty of Engineering and Information Science)

  • Wenchao Zhang

    (Central South University
    Chinese National Engineering Research Centre for Control & Treatment of Heavy Metal Pollution)

  • Jodie A. Yuwono

    (The University of Adelaide)

  • David Wexler

    (University of Wollongong, Faculty of Engineering and Information Science)

  • Yameng Fan

    (University of Wollongong, Faculty of Engineering and Information Science)

  • Jinshuo Zou

    (The University of Adelaide)

  • Gemeng Liang

    (The University of Adelaide)

  • Liang Sun

    (The University of Adelaide)

  • Zaiping Guo

    (The University of Adelaide)

Abstract

Sluggish kinetics of the CO2 reduction/evolution reactions lead to the accumulation of Li2CO3 residuals and thus possible catalyst deactivation, which hinders the long-term cycling stability of Li-CO2 batteries. Apart from catalyst design, constructing a fluorinated solid-electrolyte interphase is a conventional strategy to minimize parasitic reactions and prolong cycle life. However, the catalytic effects of solid-electrolyte interphase components have been overlooked and remain unclear. Herein, we systematically regulate the compositions of solid-electrolyte interphase via tuning electrolyte solvation structures, anion coordination, and binding free energy between Li ion and anion. The cells exhibit distinct improvement in cycling performance with increasing content of C-N species in solid-electrolyte interphase layers. The enhancement originates from a catalytic effect towards accelerating the Li2CO3 formation/decomposition kinetics. Theoretical analysis reveals that C-N species provide strong adsorption sites and promote charge transfer from interface to *CO22− during discharge, and from Li2CO3 to C-N species during charge, thereby building a bidirectional fast-reacting bridge for CO2 reduction/evolution reactions. This finding enables us to design a C-N rich solid-electrolyte interphase via dual-salt electrolytes, improving cycle life of Li-CO2 batteries to twice that using traditional electrolytes. Our work provides an insight into interfacial design by tuning of catalytic properties towards CO2 reduction/evolution reactions.

Suggested Citation

  • Fangli Zhang & Wenchao Zhang & Jodie A. Yuwono & David Wexler & Yameng Fan & Jinshuo Zou & Gemeng Liang & Liang Sun & Zaiping Guo, 2024. "Catalytic role of in-situ formed C-N species for enhanced Li2CO3 decomposition," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-47629-2
    DOI: 10.1038/s41467-024-47629-2
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