Issue 46, 2021

Redox-active zinc thiolates for low-cost aqueous rechargeable Zn-ion batteries

Abstract

Aqueous zinc-ion batteries (AZIBs) are promising candidates for large-scale electrical energy storage due to the inexpensive, safe, and non-toxic nature of zinc. One key area that requires further development is electrode materials that store Zn2+ ions with high reversibility and fast kinetics. To determine the viability of low-cost organosulfur compounds as OEMs for AZIBs, we investigate how structural modification affects electrochemical performance in Zn-thiolate complexes 1 and 2. Remarkably, modification of one thiolate in 1 to sulfide in 2 reduces the voltage hysteresis from 1.04 V to 0.15 V. While 1 exhibits negligible specific capacity due to the formation of insulating DMcT polymers, 2 delivers a capacity of 107 mA h g−1 with a primary discharge plateau at 1.1 V vs. Zn2+/Zn. Spectroscopic studies of 2 suggest a Zn2+ and H+ co-insertion mechanism with Zn2+ as the predominant charge carrier. Capacity fading in Zn-2 cells likely results from the formation of (i) soluble H+ insertion products and (ii) non-redox-active side products. Increasing electrolyte concentration and using a Nafion membrane significantly enhances the stability of 2 by suppressing H+ insertion. Our findings provide insight into the molecular design strategies to reduce the polarization potential and improve the cycling stability of the thiolate/disulfide redox couple in aqueous battery systems.

Graphical abstract: Redox-active zinc thiolates for low-cost aqueous rechargeable Zn-ion batteries

Supplementary files

Article information

Article type
Edge Article
Submitted
02 Aug. 2021
Accepted
10 Nov. 2021
First published
10 Nov. 2021
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2021,12, 15253-15262

Redox-active zinc thiolates for low-cost aqueous rechargeable Zn-ion batteries

M. R. Tuttle, C. Walter, E. Brackman, C. E. Moore, M. Espe, C. Rasik, P. Adams and S. Zhang, Chem. Sci., 2021, 12, 15253 DOI: 10.1039/D1SC04231A

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