Journal
ADVANCED MATERIALS
Volume 33, Issue 24, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202101788
Keywords
cathode design; geometric and electronic structures; K‐ ion batteries; TMO; (6) motif
Categories
Funding
- National Natural Science Foundation of China [51822210, 51972329, 22005329, 52061160484, 51802338]
- Key-Area Research and Development Program of Guangdong Province [2019B090914003]
- Shenzhen Science and Technology Planning Project [JCYJ20190807172001755, JCYJ20200109115624923, JCYJ20180507182512042]
- Guangdong Basic and Applied Basic Research Foundation [2019A1515110975, 2019TX05L389, 2018A050506066]
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The physical and chemical properties of materials are largely determined by the bonding and electronic structures of their fundamental units. A new cathode design for K-ion batteries, K2Fe(C2O4)(2), with a trigonal prism structure shows excellent electrochemical activity and cycling stability. Detailed synchrotron X-ray absorption spectroscopy measurements reveal the evolution of localized fine structures, demonstrating the electrochemical activity, reversibility, and stability of the trigonal prism motif.
The intrinsic physical and chemical properties of materials are largely governed by the bonding and electronic structures of their fundamental building units. The majority of cathode materials contain octahedral TMO6 (TM = transition metal), which dominates the redox chemistry during electrochemical operation. As a less symmetric form of TMO6, the trigonal prismatic geometry is not a traditionally favored coordination configuration as it tends to lose the crystal-field stabilization energy and thus generate large ligand repulsion. Herein, a K-ion battery cathode design, K2Fe(C2O4)(2), is shown , where the TMO6 trigonal prism (TP) is not only electrochemically active but stable enough to allow for excellent cycling stability. Detailed synchrotron X-ray absorption spectroscopy measurements reveal the evolution of localized fine structure, evidencing the electrochemical activity, reversibility, and stability of the TP motif. The findings are expected to expand the toolbox for the rational design of electrode materials by taking advantage of TP as a structural gene.
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