TY - JOUR
T1 - Enabling selective zinc-ion intercalation by a eutectic electrolyte for practical anodeless zinc batteries
AU - Li, Chang
AU - Kingsbury, Ryan
AU - Thind, Arashdeep Singh
AU - Shyamsunder, Abhinandan
AU - Fister, Timothy T.
AU - Klie, Robert F.
AU - Persson, Kristin A.
AU - Nazar, Linda F.
N1 - Funding Information:
This work was financially supported by the Joint Centre for Energy Storage Research, an Energy Innovation Hub funded by the US. Department of Energy, Office of Science, Basic Energy Sciences. We would like to thank Dr. P. Broderson (University of Toronto) for carrying out the XPS and TEM experiments, Evan Spotte-Smith (University of California, Berkeley) for assistance with DFT free energy calculations, Dr. Julian Self (University of California, Berkeley) for helpful guidance regarding charge scaling protocols for MD simulations, and Prof. A. Klinkova/Jury Medvedev (University of Waterloo) for the GC data. L.F.N also acknowledges NSERC for platform support through the Discovery Grant and Canada Research Chair programs.
Funding Information:
This work was financially supported by the Joint Centre for Energy Storage Research, an Energy Innovation Hub funded by the US. Department of Energy, Office of Science, Basic Energy Sciences. We would like to thank Dr. P. Broderson (University of Toronto) for carrying out the XPS and TEM experiments, Evan Spotte-Smith (University of California, Berkeley) for assistance with DFT free energy calculations, Dr. Julian Self (University of California, Berkeley) for helpful guidance regarding charge scaling protocols for MD simulations, and Prof. A. Klinkova/Jury Medvedev (University of Waterloo) for the GC data. L.F.N also acknowledges NSERC for platform support through the Discovery Grant and Canada Research Chair programs.
Publisher Copyright:
© 2023, The Author(s).
PY - 2023/12
Y1 - 2023/12
N2 - 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.
AB - 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.
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U2 - 10.1038/s41467-023-38460-2
DO - 10.1038/s41467-023-38460-2
M3 - Article
C2 - 37244907
AN - SCOPUS:85160251451
SN - 2041-1723
VL - 14
JO - Nature communications
JF - Nature communications
IS - 1
M1 - 3067
ER -