4.6 Article

Enhanced Oxide Reduction by Hydrogen at Cuprous Oxide-Copper Interfaces near Ascending Step Edges

Journal

JOURNAL OF PHYSICAL CHEMISTRY C
Volume -, Issue -, Pages -

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.2c03719

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Funding

  1. US Department of Energy, Division of Chemical Sciences [DE-SC0012704]
  2. U.S. DOE Office of Science Facility [DE-SC0012704]

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Understanding the dynamic processes of hydrogen interaction with oxides is crucial in catalysis. This study investigated the reduction of Cu2O-29 surfaces by hydrogen at room temperature, observing that reduction occurs preferentially at step edges and defects, with the rate depending on nearby Cu step edges. A proposed mechanism involves free copper atoms from ascending metallic step edges facilitating H2 dissociation and transfer to Cu2O regions.
Understanding the dynamic processes involved in the interaction of hydrogen with oxides is of fundamental importance in catalysis. This paper probes the reduction of Cu2O-29 surfaces by hydrogen at room temperature combining in situ ambient pressure scanning tunneling microscopy (STM), X-ray photoelectron spectroscopy (XPS), and density functional theory (DFT) calculations. Reduction of the atomic layer thin Cu2O film is observed to be preferentially initiated at step edges and terrace defects, where perfect Cu2O(111) terraces are found to be stable toward hydrogenation under the same conditions. After a long induction period, regions of partially reduced Cu2O-29 and metallic Cu coexist before the surface is fully reduced to Cu(111). The reduction rate strongly depends on the nature of nearby Cu step edges. We propose a mechanism for the reduction of Cu2O-29 by hydrogen where free copper atoms from ascending metallic step edges facilitate the formation of active ensembles for H2 dissociation and transfer H to the edges of Cu2O regions.

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