Volume 60, Issue 13 pp. 7366-7375
Research Article

Boosting Zinc Electrode Reversibility in Aqueous Electrolytes by Using Low-Cost Antisolvents

Dr. Junnan Hao

Dr. Junnan Hao

School of Chemical Engineering & Advanced Materials, The University of Adelaide, Adelaide, SA, 5005 Australia

These authors contributed equally to this work.

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Libei Yuan

Libei Yuan

Institute for Superconducting and Electronic Materials, Australian Institute for Innovative Materials, University of Wollongong, Wollongong, NSW, 2522 Australia

These authors contributed equally to this work.

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Dr. Chao Ye

Dr. Chao Ye

School of Chemical Engineering & Advanced Materials, The University of Adelaide, Adelaide, SA, 5005 Australia

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Dr. Dongliang Chao

Dr. Dongliang Chao

School of Chemical Engineering & Advanced Materials, The University of Adelaide, Adelaide, SA, 5005 Australia

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Dr. Kenneth Davey

Dr. Kenneth Davey

School of Chemical Engineering & Advanced Materials, The University of Adelaide, Adelaide, SA, 5005 Australia

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Prof. Zaiping Guo

Corresponding Author

Prof. Zaiping Guo

Institute for Superconducting and Electronic Materials, Australian Institute for Innovative Materials, University of Wollongong, Wollongong, NSW, 2522 Australia

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Prof. Shi-Zhang Qiao

Corresponding Author

Prof. Shi-Zhang Qiao

School of Chemical Engineering & Advanced Materials, The University of Adelaide, Adelaide, SA, 5005 Australia

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First published: 13 January 2021
Citations: 751

Graphical Abstract

Water activity and Zn2+ solvation in an ZnSO4 electrolyte are regulated by adding methanol as antisolvent. Methanol gradually interacts with the free and coordinated water in the Zn2+ solvation sheath in the electrolyte, to suppress side reactions and enhance the Zn2+ transference number. Concomitantly, Zn2+ deposition orientation is changed, resulting in dendrite-free Zn deposition and boosted Zn reversibility.

Abstract

Antisolvent addition has been widely studied in crystallization in the pharmaceutical industries by breaking the solvation balance of the original solution. Here we report a similar antisolvent strategy to boost Zn reversibility via regulation of the electrolyte on a molecular level. By adding for example methanol into ZnSO4 electrolyte, the free water and coordinated water in Zn2+ solvation sheath gradually interact with the antisolvent, which minimizes water activity and weakens Zn2+ solvation. Concomitantly, dendrite-free Zn deposition occurs via change in the deposition orientation, as evidenced by in situ optical microscopy. Zn reversibility is significantly boosted in antisolvent electrolyte of 50 % methanol by volume (Anti-M-50 %) even under harsh environments of −20 °C and 60 °C. Additionally, the suppressed side reactions and dendrite-free Zn plating/stripping in Anti-M-50 % electrolyte significantly enhance performance of Zn/polyaniline coin and pouch cells. We demonstrate this low-cost strategy can be readily generalized to other solvents, indicating its practical universality. Results will be of immediate interest and benefit to a range of researchers in electrochemistry and energy storage.

Conflict of interest

The authors declare no conflict of interest.

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