Wright, Matthew A., Surta, T. Wesley, Evans, Jae A., Lim, Jungwoo, Jo, Hongil, Hawkins, Cara J., Bahri, Mounib, Daniels, Luke M., Chen, Ruiyong, Zanella, Marco, and others. (2024) Accessing Mg‐Ion Storage in V 2 PS 10 via Combined Cationic‐Anionic Redox with Selective Bond Cleavage. Angewandte Chemie International Edition, . Article Number e202400837. ISSN 1521-3773. (doi:10.1002/anie.202400837) (KAR id:105459)
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| Official URL: https://doi.org/10.1002/anie.202400837 |
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Abstract
Magnesium batteries attract interest as alternative energy‐storage devices because of elemental abundance and potential for high energy density. Development is limited by the absence of suitable cathodes, associated with poor diffusion kinetics resulting from strong interactions between Mg2+ and the host structure. V2PS10 is reported as a positive electrode material for rechargeable magnesium batteries. Cyclable capacity of 100 mAh g−1 is achieved with fast Mg2+ diffusion of 7.2 × ${\times }$ 10−11–4 × ${\times }$ 10−14 cm2 s−1. The fast insertion mechanism results from combined cationic redox on the V site and anionic redox on the (S2)2− site; enabled by reversible cleavage of S−S bonds, identified by X‐ray photoelectron and X‐ray absorption spectroscopy. Detailed structural characterisation with maximum entropy method analysis, supported by density functional theory and projected density of states analysis, reveals that the sulphur species involved in anion redox are not connected to the transition metal centres, spatially separating the two redox processes. This facilitates fast and reversible Mg insertion in which the nature of the redox process depends on the cation insertion site, creating a synergy between the occupancy of specific Mg sites and the location of the electrons transferred.
| Item Type: | Article |
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| DOI/Identification number: | 10.1002/anie.202400837 |
| Additional information: | For the purpose of open access, the author has applied a CC BY public copyright licence to any Author Accepted Manuscript version arising from this submission. |
| Uncontrolled keywords: | X-ray diffraction, Diffusion kinetics, Intercalation, Anionic redox, Magnesium Batteries |
| Subjects: | Q Science |
| Divisions: | Divisions > Division of Natural Sciences > Physics and Astronomy |
| Funders: |
Engineering and Physical Sciences Research Council (https://ror.org/0439y7842)
The Faraday Institution (https://ror.org/05dt4bt98) |
| SWORD Depositor: | JISC Publications Router |
| Depositing User: | JISC Publications Router |
| Date Deposited: | 03 Apr 2024 13:31 UTC |
| Last Modified: | 05 Nov 2024 13:11 UTC |
| Resource URI: | https://kar.kent.ac.uk/id/eprint/105459 (The current URI for this page, for reference purposes) |
University of Kent Author Information
Chadwick, Alan V..
| Creator's ORCID: |
 https://orcid.org/0000-0002-6485-9207
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