Journal
CELL REPORTS PHYSICAL SCIENCE
Volume 2, Issue 10, Pages -Publisher
CELL PRESS
DOI: 10.1016/j.xcrp.2021.100592
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Funding
- National Science Foundation [DMR 1809866]
- Welch Foundation [A-1978-20190330]
- Advanced Light Source (ALS)
- Office of Science, Office of Basic Energy Sciences, U.S. Department of Energy [DE-AC02-05CH11231]
- DOE Office of Science by Brookhaven National Laboratory [DE-SC0012704]
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The research reports a topotactic chemical insertion mechanism of fluoride ions in FeSb2O4, involving synergies between iron and antimony centers. The separation of the redox center from the p-block coordination site alleviates structural strain and enables reversible diffusion of fluoride ions.
Fluoride-ion batteries are an attractive energy storage concept analogous to lithium-ion batteries but feature an inverted paradigm where anions are the principal charge carriers. Insertion hosts that can reversibly insert fluoride ions at room temperature are exceedingly sparse. Here, we report that topochemical insertion of fluoride ions in FeSb2O4 involves Fe2+/Fe3+ redox but is mediated by multi-center synergies between iron and antimony centers. Separation of the redox center from the p-block coordination site alleviates structural strain by enabling compensatory contraction and expansion of FeO6 and SbO3 polyhedra, respectively, p-block electron lone pairs play a critical role in weakening anion-lattice interactions, enabling reversible fluoride-ion diffusion across microns. The results illuminate the key principle that interactions traceable to stereoactive lone pairs can be used to mediate anion-lattice interactions and suggest that anion insertion hosts can be designed by pairing redoxactive transition metals with p-block cations bearing stereochemically active electron lone pairs.
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