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

Xu, Fang; An, Wei; Baber, Ashleigh E.; Grinter, David C.; Senanayake, Sanjaya D.; White, Michael G.; Liu, Ping; Stacchiola, Darío J.

doi:10.1021/acs.jpcc.2c03719

Title: Enhanced Oxide Reduction by Hydrogen at Cuprous Oxide–Copper Interfaces near Ascending Step Edges

Journal Article · 10 October 2022 · Journal of Physical Chemistry. C

DOI: https://doi.org/10.1021/acs.jpcc.2c03719 · OSTI ID:1900389

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Brookhaven National Laboratory (BNL), Upton, NY (United States); Stony Brook University, NY (United States); University of Texas at San Antonio, TX (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States); Shanghai University of Engineering Science (China)
Brookhaven National Laboratory (BNL), Upton, NY (United States); James Madison University, Harrisonburg, VA (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States); Stony Brook University, NY (United States)

We report that 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 initiated2 at step edges and terrace defects, where perfect Cu₂O(111) terraces are found to be stable towards hydrogenation under the same conditions. After a long induction period, regions of partially reduced Cu₂O-‘29’ and metallic Cu co-exist 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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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 1900389

Report Number(s):: BNL-223741-2022-JAAM

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 44 Vol. 126; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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