Regulating electrodeposition morphology in high-capacity aluminium and zinc battery anodes using interfacial metal–substrate bonding

Jingxu Zheng, David C. Bock, Tian Tang, Qing Zhao, Jiefu Yin, Killian R. Tallman, Garrett Wheeler, Xiaotun Liu, Yue Deng, Shuo Jin, Amy C. Marschilok, Esther S. Takeuchi, Kenneth J. Takeuchi and Lynden A. Archer ()
Additional contact information
Jingxu Zheng: Cornell University
David C. Bock: Brookhaven National Laboratory
Tian Tang: Cornell University
Qing Zhao: Robert Frederick Smith School of Chemical and Biomolecular Engineering
Jiefu Yin: Robert Frederick Smith School of Chemical and Biomolecular Engineering
Killian R. Tallman: Brookhaven National Laboratory
Garrett Wheeler: Brookhaven National Laboratory
Xiaotun Liu: Robert Frederick Smith School of Chemical and Biomolecular Engineering
Yue Deng: Cornell University
Shuo Jin: Robert Frederick Smith School of Chemical and Biomolecular Engineering
Amy C. Marschilok: Brookhaven National Laboratory
Esther S. Takeuchi: Brookhaven National Laboratory
Kenneth J. Takeuchi: State University of New York at Stony Brook
Lynden A. Archer: Cornell University

Nature Energy, 2021, vol. 6, issue 4, 398-406

Abstract: Abstract Although Li-based batteries have established a dominant role in the current energy-storage landscape, post-Li chemistries (for example, Al or Zn) are emerging as promising candidates for next-generation rechargeable batteries. Electrochemical cells using Al or Zn metal as the negative electrode are of interest for their potential low cost, intrinsic safety and sustainability. Presently, such cells are considered impractical because the reversibility of the metal anode is poor and the amount of charge stored is miniscule. Here we report that electrodes designed to promote strong oxygen-mediated chemical bonding between Al deposits and the substrate enable a fine control of deposition morphology and provide exceptional reversibility (99.6–99.8%). The reversibility is sustained over unusually long cycling times (>3,600 hours) and at areal capacities up to two orders of magnitude higher than previously reported values. We show that these traits result from the elimination of fragile electron transport pathways, and the non-planar deposition of Al via specific metal–substrate chemical bonding.

Date: 2021
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DOI: 10.1038/s41560-021-00797-7

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