Microscopic Investigation of H2 Reduced CuOx/Cu(111) and ZnO/CuOx/Cu(111) Inverse Catalysts: STM, AP-XPS, and DFT Studies

Mehar, Vikram; Huang, Erwei; Shi, Rui; Rui, Ning; Rosales, Rina; Waluyo, Iradwikanari; Hunt, Adrian; Liu, Ping; Rodriguez, José A.

doi:10.1021/acscatal.3c02514

Title: Microscopic Investigation of H₂ Reduced CuO_x/Cu(111) and ZnO/CuO_x/Cu(111) Inverse Catalysts: STM, AP-XPS, and DFT Studies

Journal Article · Wed Jul 12 00:00:00 EDT 2023 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.3c02514· OSTI ID:1997931

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^[1]; Rosales, Rina ^[2];

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Brookhaven National Laboratory (BNL), Upton, NY (United States)
Stony Brook Univ., NY (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Brookhaven National Laboratory (BNL), Upton, NY (United States); Stony Brook Univ., NY (United States)

Understanding the reduction mechanism of ZnO/CuO_x interfaces by hydrogen is of great importance for advancing the performance of industrial catalysts for CO₂ hydrogenation to methanol. Here, the reduction of pristine and ZnO-modified CuO_x/Cu(111) by H₂ was investigated using ambient pressure scanning tunnelling microscopy (AP-STM), ambient pressure X-ray photoelectron spectroscopy (AP-XPS) and density functional theory (DFT). The morphological changes and reaction rates seen for the reduction of CuO_x/Cu(111) and ZnO/CuO_x/Cu(111) are very different. On CuO_x/Cu(111), perfect "44" and "29" structures displayed a very low reactivity towards H₂ at room temperature. A long induction period associated with an autocatalytic process was observed to enable the reduction by the removal of chemisorbed non-lattice oxygen initially and lattice oxygen sequentially at the CuO_x-Cu interface, which led to formation of oxygen deficient "5-7" hex and honeycomb structures. In the final stages of the reduction process, regions of residual oxygen species and metallic Cu were seen. The addition of ZnO particles to CuO_x/Cu(111) opened new reaction channels. On the ZnO sites, the dissociation of H₂ was fast and H adatoms easily migrated to adjacent regions of copper oxide. This hydrogen spillover substantially enhanced the rate of oxygen removal, resulting in the rapid reduction of the copper oxide located in the periphery of the zinc oxide islands with no signs for the reduction of ZnO. The deposited ZnO completely modified the dynamics for H₂ dissociation and hydrogen migration, providing an excellent source for CO₂ hydrogenation processes on the inverse oxide/metal system.

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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). Scientific User Facilities (SUF)

Grant/Contract Number:: SC0012704; AC02-05CH11231; BNL-FWP CO-060; BNL-FWP CO-040

OSTI ID:: 1997931

Report Number(s):: BNL-224757-2023-JAAM

Journal Information:: ACS Catalysis, Vol. 13, Issue 14; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
zinc oxide
copper oxide
hydrogen
CO2 hydrogenation
H2 activation
H spillover
inverse ZnO/Cu catalysts
morphological studies
dissociation
oxides
oxygen
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scanning tunneling microscopy

Title: Microscopic Investigation of H2 Reduced CuOx/Cu(111) and ZnO/CuOx/Cu(111) Inverse Catalysts: STM, AP-XPS, and DFT Studies

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Title: Microscopic Investigation of H₂ Reduced CuO_x/Cu(111) and ZnO/CuO_x/Cu(111) Inverse Catalysts: STM, AP-XPS, and DFT Studies