Journal
CHEMICAL SCIENCE
Volume 11, Issue 17, Pages 4450-4455Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0sc01401j
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Funding
- Ulm University
- Helmholtz-Gemeinschaft (HGF)
- Deutsche Forschungsgemeinschaft (DFG) [STR1164/12, STR1164/14, TRR234, 364549901, EXC-2154/1]
- Fonds der Chemischen Industrie (FCI)
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Polyoxometalates are key materials for energy conversion and storage due to their unique chemical tunability and electrochemical reactivity. Herein, we report that functionalization of molecular vanadium oxides, polyoxovanadates, with redox-inert Ca2+ cations leads to a significant increase in their electron storage capabilities. The electrochemical performance of the Ca2+-functionalized dodecavanadate [Ca2V12O32Cl(DMF)(3)](2-) (={Ca2V12}) was thus compared with that of the precursor compound (H2NMe2)(2)[V12O32Cl](3-) (={V-12}). {Ca2V12} can store up to five electrons per cluster, while {V-12} only shows one reversible redox transition. In initial studies, we demonstrated that {Ca2V12} can be used as an active material in lithium-ion cathodes. Our results show how redox-inert cations can be used as structural and electrostatic stabilizers, leading to major changes in the redox-chemistry of polyoxovanadates.
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