Abstract
Aqueous rechargeable zinc metal batteries promise attractive advantages including safety, high volumetric energy density and low cost; however, such benefits cannot be unlocked unless Zn reversibility meets stringent commercial viability1-2.In this work, we report remarkable improvements on Zn reversibility in aqueous electrolytes when phosphonium-based cations are used to reshape interfacial structures and interphasial chemistries, particularly when their ligands contain ether linkage. This novel aqueous electrolyte supports unprecedented Zn reversibility by showing dendrite-free Zn plating/stripping for over 6400 h at 0.5 mA cm–2,or over 280 h at 2.5 mA cm–2, with coulombic efficiency above 99% even with 20% Zn utilization per-cycle. Excellent full cell performance is demonstrated with Na2V6O16·1.63H2O cathode, which cycles for 2000 times at 300 mA g–1. The microscopic characterization and modeling identify the mechanism of unique interphase chemistry from phosphonium and its functionalities as the key factors responsible for dictating reversible Zn chemistry.Reference L. E. Blanc, D. Kundu, L. F. Nazar, Joule 2020, 4, 771–799.L. Ma, M. A. Schroeder, O. Borodin, T. P. Pollard, M. S. Ding, C. Wang, K. Xu, Nature Energy 2020, 5, 743-749. Figure 1
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