期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 28, 页码 11483-11490出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202002560
关键词
anions; magnesium-ion batteries; multi-electron reactions; rechargeable calcium batteries; VS4
资金
- Bundesministerium fr Bildung und Forschung (BMBF) of Germany [03XP0208]
- European Unions Horizon 2020 research and innovation programme via the E-MAGIC project [824066]
- German Research Foundation (DFG) [390874152]
- Karlsruhe Nano Micro Facility (KNMF), a Helmholtz Research Infrastructure at Karlsruhe Institute of Technology (KIT)
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.
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