Cation replacement method enables high-performance electrolytes for multivalent metal batteries

Siyuan Li, Jiahui Zhang, Shichao Zhang, Qilei Liu, Hao Cheng, Lei Fan, Weidong Zhang, Xinyang Wang, Qian Wu and Yingying Lu ()
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Siyuan Li: Zhejiang University
Jiahui Zhang: Zhejiang University
Shichao Zhang: Zhejiang University
Qilei Liu: State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, Institute of Chemical Process Systems Engineering, School of Chemical Engineering, Dalian University of Technology
Hao Cheng: Zhejiang University
Lei Fan: Zhejiang University
Weidong Zhang: Zhejiang University
Xinyang Wang: Zhejiang University
Qian Wu: Zhejiang University
Yingying Lu: Zhejiang University

Nature Energy, 2024, vol. 9, issue 3, 285-297

Abstract: Abstract High-performance, cost-efficient electrolyte systems are sought after for high-energy-density multivalent metal batteries. However, the expensive precursor and complex synthesis process hinders exploration of cathode electrode/electrolyte interfaces and solvation structures. Here we developed a universal cation replacement method to prepare low-cost, high-reversibility magnesium and calcium electrolytes derived from a zinc organoborate solvation structure. By rationally adjusting the precursor chain length and F-substitution degree, we can fine tune anion participation in the primary solvation shell. A completely dissociated Mg organoborate electrolyte enables high current endurance and enhanced electrochemical kinetics, whereas the Ca organoborate electrolyte with strong coordination/B–H inclusion offers a stable solid–electrolyte interphase with high coulombic efficiency. A rechargeable 53.4 Wh kg−1 Mg metal prototype is achieved with a 30 μm Mg anode, a low electrolyte/sulfur ratio (E/S = 5.58 μl mg−1) and a modified separator/interlayer. This work provides innovative strategies for reversible electrolyte systems and high-energy-density multivalent metal batteries.

Date: 2024
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DOI: 10.1038/s41560-023-01439-w

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