Nonpolarizing oxygen-redox capacity without O-O dimerization in Na2Mn3O7

Akihisa Tsuchimoto, Xiang-Mei Shi, Kosuke Kawai, Benoit Mortemard de Boisse, Jun Kikkawa, Daisuke Asakura, Masashi Okubo and Atsuo Yamada ()
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Akihisa Tsuchimoto: The University of Tokyo
Xiang-Mei Shi: The University of Tokyo
Kosuke Kawai: The University of Tokyo
Benoit Mortemard de Boisse: The University of Tokyo
Jun Kikkawa: National Institute for Materials Science (NIMS)
Daisuke Asakura: National Institute of Advanced Industrial Science and Technology (AIST)
Masashi Okubo: The University of Tokyo
Atsuo Yamada: The University of Tokyo

Nature Communications, 2021, vol. 12, issue 1, 1-7

Abstract: Abstract Reversibility of an electrode reaction is important for energy-efficient rechargeable batteries with a long battery life. Additional oxygen-redox reactions have become an intensive area of research to achieve a larger specific capacity of the positive electrode materials. However, most oxygen-redox electrodes exhibit a large voltage hysteresis >0.5 V upon charge/discharge, and hence possess unacceptably poor energy efficiency. The hysteresis is thought to originate from the formation of peroxide-like O22− dimers during the oxygen-redox reaction. Therefore, avoiding O-O dimer formation is an essential challenge to overcome. Here, we focus on Na2-xMn3O7, which we recently identified to exhibit a large reversible oxygen-redox capacity with an extremely small polarization of 0.04 V. Using spectroscopic and magnetic measurements, the existence of stable O−• was identified in Na2-xMn3O7. Computations reveal that O−• is thermodynamically favorable over the peroxide-like O22− dimer as a result of hole stabilization through a (σ + π) multiorbital Mn-O bond.

Date: 2021
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DOI: 10.1038/s41467-020-20643-w

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