Ultrafast Metal Electrodeposition Revealed by In Situ Optical Imaging and Theoretical Modeling towards Fast-Charging Zn Battery Chemistry

Zhao Cai; Jindi Wang; Ziheng Lu; Renming Zhan; Yangtao Ou; Li Wang; Mouad Dahbi; Jones Alami; Jun Lu; Khalil Amine; Yongming Sun

doi:10.1002/anie.202116560

Ultrafast Metal Electrodeposition Revealed by In Situ Optical Imaging and Theoretical Modeling towards Fast-Charging Zn Battery Chemistry

Angew Chem Int Ed Engl. 2022 Mar 28;61(14):e202116560. doi: 10.1002/anie.202116560. Epub 2022 Feb 10.

Authors

Zhao Cai¹, Jindi Wang¹, Ziheng Lu², Renming Zhan¹, Yangtao Ou¹, Li Wang³, Mouad Dahbi⁴, Jones Alami⁴, Jun Lu⁵, Khalil Amine^{5

6}, Yongming Sun¹

Affiliations

¹ Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan, 430074, China.
² Department of Materials Science and Metallurgy, University of Cambridge, Cambridge, CB3 0FS, United Kingdom.
³ Institute of Nuclear & New Energy Technology, Tsinghua University, Beijing, 100084, China.
⁴ Materials Science and Nano-Engineering Department, Mohammed VI Polytechnic University, Ben Guerir, Morocco.
⁵ Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, 60439, USA.
⁶ Department of Material Science and Engineering, Stanford University, Stanford, CA 94305, USA.

PMID: 35088500
DOI: 10.1002/anie.202116560

Abstract

Metallic Zn is a preferred anode material for rechargeable aqueous batteries towards a smart grid and renewable energy storage. Understanding how the metal nucleates and grows at the aqueous Zn anode is a critical and challenging step to achieve full reversibility of Zn battery chemistry, especially under fast-charging conditions. Here, by combining in situ optical imaging and theoretical modeling, we uncover the critical parameters governing the electrodeposition stability of the metallic Zn electrode, that is, the competition among crystallographic thermodynamics, kinetics, and Zn²⁺ -ion diffusion. Moreover, steady-state Zn metal plating/stripping with Coulombic efficiency above 99 % is achieved at 10-100 mA cm^-2 in a reasonably high concentration (3 M) ZnSO₄ electrolyte. Significantly, a long-term cycling-stable Zn metal electrode is realized with a depth of discharge of 66.7 % under 50 mA cm^-2 in both Zn||Zn symmetrical cells and MnO₂ ||Zn full cells.

Keywords: Aqueous Battery; Electrodeposition; Fast-Charging; Reversibility; Zn Anode.