Affiliation:
1. State Key Lab of Organic-Inorganic Composites, Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology Beijing 100029 People's Republic of China
2. Dongying Industrial Product Inspection & Metrology Verification Center Dongying 257000 People's Republic of China
3. School of Mechanical and Manufacturing Engineering University of New South Wales Sydney, New South Wales 2052 Australia
Abstract
AbstractTransition 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 MnO2, yielding N‐coordinated MnO2 (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 eg orbitals. The resultant TEAMO exhibit a significant increase in storage capacity, reaching 351 mAh g−1 at 0.1 A g−1. Our findings suggest a viable strategy for optimizing the electronic structure of TMO cathodes, enhancing the potential of ZIBs in energy storage technology.
Funder
National Natural Science Foundation of China