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pH-Triggered Molecular Switch Toward Texture-Regulated Zn Anode
Authors:Shao-Jian Zhang  Dr Junnan Hao  Yilong Zhu  Dr Huan Li  Prof Zhan Lin  Prof Shi-Zhang Qiao
Institution:1. School of Chemical Engineering & Advanced Materials, The University of Adelaide, Adelaide, SA-5005 Australia

These authors contributed equally to this work.;2. School of Chemical Engineering & Advanced Materials, The University of Adelaide, Adelaide, SA-5005 Australia;3. Guangdong Provincial Key Laboratory of Plant Resources Biorefinery, School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou, 510006 China

Abstract:Zn electrodes in aqueous media exhibit an unstable Zn/electrolyte interface due to severe parasitic reactions and dendrite formation. Here, a dynamic Zn interface modulation based on the molecular switch strategy is reported by hiring γ-butyrolactone (GBL) in ZnCl2/H2O electrolyte. During Zn plating, the increased interfacial alkalinity triggers molecular switch from GBL to γ-hydroxybutyrate (GHB). GHB strongly anchors on Zn surface via triple Zn−O bonding, leading to suppressive hydrogen evolution and texture-regulated Zn morphology. Upon Zn stripping, the fluctuant pH turns the molecular switch reaction off through the cyclization of GHB to GBL. This dynamic molecular switch strategy enables high Zn reversibility with Coulombic efficiency of 99.8 % and Zn||iodine batteries with high-cyclability under high Zn depth of discharge (50 %). This study demonstrates the importance of dynamic modulation for Zn electrode and realizes the reversible molecular switch strategy to enhance its reversibility.
Keywords:Dynamic Interface  High Zn DOD  Low Temperature  Molecular Switch  Zn-Ion Battery
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