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Functionalized Phosphonium Cations Enable Zinc Metal Reversibility in Aqueous Electrolytes
Author(s) -
Ma Lin,
Pollard Travis P.,
Zhang Yong,
Schroeder Marshall A.,
Ding Michael S.,
Cresce Arthur V.,
Sun Ruimin,
Baker David R.,
Helms Brett A.,
Maginn Edward J.,
Wang Chunsheng,
Borodin Oleg,
Xu Kang
Publication year - 2021
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.202017020
Subject(s) - phosphonium , faraday efficiency , chemistry , aqueous solution , electrolyte , zinc , inorganic chemistry , stripping (fiber) , metal , chemical engineering , materials science , organic chemistry , electrode , engineering , composite material
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 viability. Herein, 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 an 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 Na 2 V 6 O 16 ⋅1.63 H 2 O 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