Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 12, Issue 24, Pages 5675-5681Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.1c01422
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Funding
- Basic Science Center Project of the National Natural Science Foundation of China [51788104]
- National Natural Science Foundation of China [51525102, 51371102, 51390475, 51761135131]
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The atomic structures of the (101) and (001) surfaces of Mn3O4 have been determined, showing that the (101) surface undergoes subsurface reconstruction while the (001) surface has Mn(III) ions in the outermost layer. These findings provide a microscopic understanding of the higher catalytic activity of the (001) surface compared to the (101) surface and could lead to the development of novel catalysts based on Mn3O4.
The Mn(III) ions at Mn3O4 surface are hypothesized to contribute to catalytic activity in oxygen reduction reaction. However, the surface structure and stability of Mn3O4 are far less understood. Here, the atomic structures of the widespread (101) and (001) surfaces of Mn3O4 are determined by combining aberration-corrected transmission electron microscopy and DFT calculations. The surface stabilization mechanisms and the oxidation states of Mn are revealed and correlated to the catalytic activity of the surfaces. The results show that the (101) surface undergoes a subsurface reconstruction, forming a rock-salt-type surface layer. The Mn(III) ions are in the outermost layer of the (001) surface but in the subsurface of the (101) surface. The surface partition of the Mn(III) ions provides a microscopic understanding to the observed higher catalytic activity of the (001) surface relative to the (101) surface and would contribute to further development of novel catalysts based on Mn3O4.
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