The electrolyte comprising more robust water and superhalides transforms Zn‐metal anode reversibly and dendrite‐free
Chong Zhang,
Woochul Shin,
Liangdong Zhu,
Cheng Chen,
Joerg C. Neuefeind,
Yunkai Xu,
Sarah I. Allec,
Cong Liu,
Zhixuan Wei,
Aigerim Daniyar,
Jia‐Xing Jiang,
Chong Fang,
P. Alex Greaney,
Xiulei Ji
Affiliations
Chong Zhang
Key Laboratory of Applied Surface and Colloid Chemistry (Shaanxi Normal University), Ministry of Education, Shaanxi Key Laboratory for Advanced Energy Devices, School of Materials Science and Engineering Shaanxi Normal University Xi'an Shaanxi China
Woochul Shin
Department of Chemistry Oregon State University Corvallis Oregon
Liangdong Zhu
Department of Chemistry Oregon State University Corvallis Oregon
Cheng Chen
Department of Chemistry Oregon State University Corvallis Oregon
Joerg C. Neuefeind
Spallation Neutron Source Oak Ridge National Laboratory Oak Ridge Tennessee
Yunkai Xu
Department of Chemistry Oregon State University Corvallis Oregon
Sarah I. Allec
Materials Science and Engineering University of California Riverside California
Cong Liu
Argonne National Laboratory Chemical Sciences and Engineering Division Lemont Illinois
Zhixuan Wei
Department of Chemistry Oregon State University Corvallis Oregon
Aigerim Daniyar
Department of Chemistry Oregon State University Corvallis Oregon
Jia‐Xing Jiang
Key Laboratory of Applied Surface and Colloid Chemistry (Shaanxi Normal University), Ministry of Education, Shaanxi Key Laboratory for Advanced Energy Devices, School of Materials Science and Engineering Shaanxi Normal University Xi'an Shaanxi China
Chong Fang
Department of Chemistry Oregon State University Corvallis Oregon
P. Alex Greaney
Materials Science and Engineering University of California Riverside California
Xiulei Ji
Department of Chemistry Oregon State University Corvallis Oregon
Abstract A great challenge for all aqueous batteries, including Zn‐metal batteries, is the parasitic hydrogen evolution reaction on the low‐potential anode. Herein, we report the formula of a highly concentrated aqueous electrolyte that mitigates hydrogen evolution by transforming water molecules more inert. The electrolyte comprises primarily ZnCl2 and LiCl as an additive, both of which are inexpensive salts. The O–H covalent bonds in water get strengthened in a chemical environment that has fewer hydrogen bonding interactions and a greater number of Zn–Cl superhalides, as suggested by integrated characterization and simulation. As a result, the average Coulombic efficiency of zinc‐metal anode is raised to an unprecedented >99.7% at 1 mA cm−2. In the new electrolyte, the plating/stripping processes leave the zinc‐metal anode dendrite‐free, and the zinc‐metal anode delivers stable plating/stripping cycles for 4000 hours with an areal capacity of 4 mAh cm−2 at 2 mA cm−2. Furthermore, the high Coulombic efficiency of zinc‐metal anode in the ZnCl2‐LiCl mixture electrolyte is demonstrated in full cells with a limited anode. The V2O5·H2O||Zn full cell with an N/P mass ratio of 1.2 delivers a stable life of more than 2500 cycles, and the LiMn2O4||Zn hybrid cell with an N/P mass ratio of 0.6 exhibits 1500 cycles in its stable life.
