Preparation and Structural Characterization of ZrO2/CuOx/Cu(111) Inverse Model Catalysts

Shi, Rui; Mahapatra, Mausumi; Kang, Jindong; Orozco, Ivan; Senanayake, Sanjaya D.; Rodriguez, José A.

doi:10.1021/acs.jpcc.0c00852

Title: Preparation and Structural Characterization of ZrO₂/CuO_x/Cu(111) Inverse Model Catalysts

Journal Article · Fri Apr 17 00:00:00 EDT 2020 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.0c00852· OSTI ID:1617683

Shi, Rui ^[1];

^[2]; Kang, Jindong ^[1]; Orozco, Ivan ^[1];

^[2];

^[3]

State Univ. of New York (SUNY), Stony Brook, NY (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
State Univ. of New York (SUNY), Stony Brook, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)

CO₂ hydrogenation to methanol is regarded as a promising reaction to catalytically convert a major greenhouse gas (CO₂) into a value-added product (methanol). In the current study, scanning tunneling microscopy (STM) and X-ray photoelectron spectroscopy (XPS) were applied to investigate the growth mode of low coverages (<0.2 ML) of ZrO₂ in an inverse ZrO₂/CuOx/Cu(111) system, which has the potential to achieve a high selectivity for a direct CO₂ to methanol transformation. It was found that the morphology of ZrO₂ was strongly affected by the preparation method. The ZrO₂/CuO_x/Cu(111) model catalyst prepared by the oxidation at 600 K of Zr pre-deposited on Cu(111) exhibited substantial mixing of ZrO₂ and CuO_x. In contrast, the direct deposition of Zr under an O₂ ambient over CuO_x/Cu(111) at 600 K produced small ZrO₂ islands (10-12 nm in size) with a two-dimensional structure (i.e. only one layer of ZrO₂). XPS studies indicate that both preparation methods lead to ZrO₂/CuO_x/Cu(111) surfaces. The model catalyst prepared by the direct deposition of Zr in O₂ was annealed up to 700 K in ultra-high vacuum. Both STM and XPS results suggest no apparent change in ZrO₂, while CuO_x was reduced at such annealing conditions. The island size of 10-12 nm observed for ZrO₂ on Cu(111) is much smaller than island sizes seen for CeO₂ (30-50 nm) and ZnO (300-500 nm) on the same substrate, opening the possibility for unique chemical properties

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Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States)

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

Grant/Contract Number:: SC0012704

OSTI ID:: 1617683

Report Number(s):: BNL-215909-2020-JAAM

Journal Information:: Journal of Physical Chemistry. C, Vol. 124, Issue 19; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 9 works

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