Transition metal oxides (TMOs) are promising cathode materials for aqueous zinc ion batteries (ZIBs), however, their performance is hindered by a substantial Hubbard gap, which limits electron transfer and battery cyclability. Addressing this, we introduce a heteroatom coordination approach, using triethanolamine to induce axial N coordination on Mn centers in MnO, yielding N-coordinated MnO (TEAMO). This approach leverages the change of electronegativity disparity between Mn and ligands (O and N) to disrupt spin symmetry and augment spin polarization. This enhancement leads to the closure of the Hubbard gap, primarily driven by the intensified occupancy of the Mn e orbitals. The resultant TEAMO exhibit a significant increase in storage capacity, reaching 351 mAh g at 0.1 A g. Our findings suggest a viable strategy for optimizing the electronic structure of TMO cathodes, enhancing the potential of ZIBs in energy storage technology.
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http://dx.doi.org/10.1002/anie.202408414 | DOI Listing |
Dalton Trans
December 2024
Department of Science and High Technology - Insubria University and INSTM, Via Valleggio 11, 22100 Como, Italy.
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Wageningen Livestock Research, Wageningen University & Research, Wageningen, Netherlands.
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View Article and Find Full Text PDFJ Phys Condens Matter
December 2024
Department of Physics, Indian Institute of Technology Roorkee, Roorkee 247667, Uttarakhand, India.
Chem Mater
November 2024
Department of Materials, Oxford University, Oxford OX1 3PH, U.K.
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Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, 94720, CA, USA.
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