Spin Symmetry Breaking-Induced Hubbard Gap Near-Closure in N-Coordinated MnO for Enhanced Aqueous Zinc-Ion Battery Performance.

Angew Chem Int Ed Engl

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.

Published: August 2024

AI Article Synopsis

  • Transition metal oxides (TMOs) face performance issues in aqueous zinc ion batteries (ZIBs) due to a significant Hubbard gap that limits electron transfer.
  • To overcome this, researchers developed a method using triethanolamine to create N-coordinated MnO (TEAMO), which alters the electronic properties of manganese.
  • The enhancement in spin polarization and the closure of the Hubbard gap significantly improve the storage capacity of TEAMO to 351 mAh/g at 0.1 A/g, presenting a promising strategy for boosting TMO cathodes in energy storage applications.

Article Abstract

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.202408414DOI Listing

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