Issue 20, 2022

Multivalent cationic and anionic mixed redox of an Sb2S3 cathode toward high-capacity aluminum ion batteries

Abstract

The conventional cationic redox centers of transition-metal-based cathodes are reaching their theoretical capacity limit, which cannot match the ultra-high specific capacity contributed by the three-electron transfer reaction of an Al anode (2980 mA h g−1, 8056 mA h cm−3), severely restraining the development of high-energy rechargeable Al-ion batteries (RAIBs). In this work, we propose the multivalent cationic and anionic mixed redox chemistry of Sb2S3 as a promising way out of this problem. The energy storage is induced by the cumulative Sb-related cationic (Sb(+3) ⇔ Sb(+5)) and S-related anionic (S(−2) ⇔ S(0)) mixed 10-electron transfer reversible redox reaction during the charge/discharge process, which has been elucidated here by extensive electrochemical measurements and characterizations. Furthermore, excellent electrochemical performances are realized due to the carbon-based interlayer effectively blocking the charging products of the Sb-based cationic cluster (SbCl4+), by a dual defense mechanism that integrates the physical barrier of the porous structure and the powerful chemical adsorption ability of the oxygen groups. The Sb2S3 cathode could deliver a discharge specific capacity of 756 mA h g−1 at 100 mA g−1. The finding is that the joint multivalent cationic and anionic redox chemistry proposed in this work opens up new opportunities for designing high-performance electrodes for advanced rechargeable batteries.

Graphical abstract: Multivalent cationic and anionic mixed redox of an Sb2S3 cathode toward high-capacity aluminum ion batteries

Supplementary files

Article information

Article type
Communication
Submitted
16 mar 2022
Accepted
21 apr 2022
First published
21 apr 2022

J. Mater. Chem. A, 2022,10, 10829-10836

Multivalent cationic and anionic mixed redox of an Sb2S3 cathode toward high-capacity aluminum ion batteries

T. Li, T. Cai, H. Hu, X. Li, D. Wang, Y. Zhang, Y. Cui, L. Zhao, W. Xing and Z. Yan, J. Mater. Chem. A, 2022, 10, 10829 DOI: 10.1039/D2TA02049A

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