Multi-Electron Reactions enabled by Anion-Based Redox Chemistry for High-Energy Multivalent Rechargeable Batteries
Authors:
- Z. Li,
- Bhaghavathi P. Vinayan,
- Piotr Jankowski,
- Christian Njel,
- Ananyo Roy,
- Tejs Vegge,
- Julia Maibach,
- Juan Maria García Lastra,
- Maximilian Fichtner,
- Zhirong Zhao-Karger
Abstract
The development of multivalent metal (such as Mg and Ca) based battery systems is hindered by lack of suitable cathode chemistry that shows reversible multi-electron redox reactions. Cationic redox centres in the classical cathodes can only afford stepwise single-electron transfer, which are not ideal for multivalent-ion storage. The charge imbalance during multivalent ion insertion might lead to an additional kinetic barrier for ion mobility. Therefore, multivalent battery cathodes only exhibit slope-like voltage profiles with insertion/extraction redox of less than one electron. Taking VS4 as a model material, reversible two-electron redox with cationic–anionic contributions is verified in both rechargeable Mg batteries (RMBs) and rechargeable Ca batteries (RCBs). The corresponding cells exhibit high capacities of >300 mAh g−1 at a current density of 100 mA g−1 in both RMBs and RCBs, resulting in a high energy density of >300 Wh kg−1 for RMBs and >500 Wh kg−1 for RCBs. Mechanistic studies reveal a unique redox activity mainly at anionic sulfides moieties and fast Mg2+ ion diffusion kinetics enabled by the soft structure and flexible electron configuration of VS4.
- Record ID
- WUT3bf1e5c58e91498e97fbb376b77739f0
- Author
- Journal series
- Angewandte Chemie-International Edition, ISSN 1433-7851, e-ISSN 1521-3773
- Issue year
- 2020
- Vol
- 59
- Pages
- 11483-11490
- Publication size in sheets
- 574.15
- ASJC Classification
- ;
- DOI
- DOI:10.1002/anie.202002560 Opening in a new tab
- URL
- https://onlinelibrary.wiley.com/doi/full/10.1002/anie.202002560 Opening in a new tab
- Language
- (en) English
- File
-
- File: 1
- anie.202002560.pdf
-
- Score (nominal)
- 200
- Score source
- journalList
- Score
- = 200.0, 13-05-2022, ArticleFromJournal
- Publication indicators
- = 40; : 2018 = 2.132; : 2020 (2 years) = 15.336 - 2020 (5 years) =14.205
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- Uniform Resource Identifier
- https://repo.pw.edu.pl/info/article/WUT3bf1e5c58e91498e97fbb376b77739f0/
- URN
urn:pw-repo:WUT3bf1e5c58e91498e97fbb376b77739f0
* presented citation count is obtained through Internet information analysis and it is close to the number calculated by the Publish or PerishOpening in a new tab system.