Enabling selective zinc-ion intercalation by a eutectic electrolyte for practical anodeless zinc batteries

Chang Li, Ryan Kingsbury, Arashdeep Singh Thind, Abhinandan Shyamsunder, Timothy T. Fister, Robert F. Klie, Kristin A. Persson () and Linda F. Nazar ()
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Chang Li: University of Waterloo
Ryan Kingsbury: Lawrence Berkeley National Laboratory
Arashdeep Singh Thind: Argonne National Laboratory
Abhinandan Shyamsunder: University of Waterloo
Timothy T. Fister: Argonne National Laboratory
Robert F. Klie: Argonne National Laboratory
Kristin A. Persson: Argonne National Laboratory
Linda F. Nazar: University of Waterloo

Nature Communications, 2023, vol. 14, issue 1, 1-13

Abstract: Abstract Two major challenges hinder the advance of aqueous zinc metal batteries for sustainable stationary storage: (1) achieving predominant Zn-ion (de)intercalation at the oxide cathode by suppressing adventitious proton co-intercalation and dissolution, and (2) simultaneously overcoming Zn dendrite growth at the anode that triggers parasitic electrolyte reactions. Here, we reveal the competition between Zn2+ vs proton intercalation chemistry of a typical oxide cathode using ex-situ/operando techniques, and alleviate side reactions by developing a cost-effective and non-flammable hybrid eutectic electrolyte. A fully hydrated Zn2+ solvation structure facilitates fast charge transfer at the solid/electrolyte interface, enabling dendrite-free Zn plating/stripping with a remarkably high average coulombic efficiency of 99.8% at commercially relevant areal capacities of 4 mAh cm−2 and function up to 1600 h at 8 mAh cm−2. By concurrently stabilizing Zn redox at both electrodes, we achieve a new benchmark in Zn-ion battery performance of 4 mAh cm−2 anode-free cells that retain 85% capacity over 100 cycles at 25 °C. Using this eutectic-design electrolyte, Zn | |Iodine full cells are further realized with 86% capacity retention over 2500 cycles. The approach represents a new avenue for long-duration energy storage.

Date: 2023
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DOI: 10.1038/s41467-023-38460-2

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