Issue 11, 2022

Unveiling solvation structure and desolvation dynamics of hybrid electrolytes for ultralong cyclability and facile kinetics of Zn–Al alloy anodes

Abstract

Despite the high theoretical capacity and natural abundance of Al metal anodes, the reversible and fast multivalent storage of Al3+ ions remains challenging because their large charge density leads to strong electrostatic interactions with other components and sluggish kinetics. Herein, we report the record-high plating/stripping time (>8000 h) and high rate capability of Zn–Al alloy anodes in Al3+-containing hybrid electrolytes. The more reversible Al deposition on Zn in nitrile-based hybrid electrolyte than carbonate- and amide-based hybrid and aqueous electrolytes is attributed to weak Al3+–solvent interactions and fast Al3+ transfer kinetics. In particular, these electrochemical behaviors of nitrile-based electrolyte originate from a unique solvation structure, the interrelation among H2O, organic solvents, and Al3+, and the conformational change of bound/free solvents upon desolvation, as elaborated via theoretical simulations, two-dimensional infrared correlation spectroscopy, and other characterizations. The superiority of this hybrid electrolyte was confirmed by achieving a high specific capacity (183 mA h g−1 and 1.08 mA h cm−2) and long cycling of >5000 cycles of full cells integrating Zn–Al alloy anodes (25 μm) with vanadium dioxide/carbon nanotubes (8 mg cm−2) and activated carbon (10 mg cm−2) cathodes, respectively, which considerably exceed those of Al-based full cells.

Graphical abstract: Unveiling solvation structure and desolvation dynamics of hybrid electrolytes for ultralong cyclability and facile kinetics of Zn–Al alloy anodes

Supplementary files

Article information

Article type
Paper
Submitted
31 جوٗلایی 2022
Accepted
09 ستمبر 2022
First published
15 ستمبر 2022

Energy Environ. Sci., 2022,15, 4572-4583

Unveiling solvation structure and desolvation dynamics of hybrid electrolytes for ultralong cyclability and facile kinetics of Zn–Al alloy anodes

Q. Dou, N. Yao, W. K. Pang, Y. Park, P. Xiong, X. Han, H. H. Rana, X. Chen, Z. Fu, L. Thomsen, B. Cowie, Y. Kang, Q. Liu, D. H. Min, Y. M. Jung, Z. Guo, Q. Zhang and H. S. Park, Energy Environ. Sci., 2022, 15, 4572 DOI: 10.1039/D2EE02453E

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements