Promoting effect of tungsten carbide on the catalytic activity of Cu for CO2 reduction

Koverga, Andrey A.; Flórez, Elizabeth; Dorkis, Ludovic; Rodriguez, José A.

doi:10.1039/d0cp00358a

Title: Promoting effect of tungsten carbide on the catalytic activity of Cu for CO2 reduction

Journal Article · Wed Jan 01 00:00:00 EST 2020 · Physical Chemistry Chemical Physics. PCCP (Print)

DOI:https://doi.org/10.1039/d0cp00358a· OSTI ID:1642410

^[1];

^[2]; Dorkis, Ludovic ^[1];

^[3]

Univ. Nacional de Colombia, Medellin (Colombia); Univ. de Medellin (Colombia)
Univ. de Medellin (Colombia)
Brookhaven National Lab. (BNL), Upton, NY (United States)

In this work, the adsorption of H, CO₂, HCOO, O and CO on copper monolayers and submonolayers supported on hexagonal WC(0001) surfaces has been investigated. Calculations have been performed using density functional theory with the Perdew–Burke–Ernzerhof exchange correlation functional and D2 van der Waals corrections. Additionally, dipole corrections were also included. The catalytic properties of supported Cu on both carbon- and metal-terminated WC(0001) surfaces were explored. On carbon-terminated WC(0001) surfaces, Cu tends to be oxidized, while on the metallic terminated surface, it gains charge. The results indicate that all studied Cu/WC(0001) surfaces bind all adsorbates stronger than the extended Cu(111). For CO, the binding energy is so large in some cases (1.6–2.2 eV) that it could potentially lead to catalyst deactivation. Nevertheless, surfaces with an adsorbed Cu monolayer, Cu_ML, are less prone to this deactivation, since there are not WC surface atoms; and thus, the contribution of strong CO adsorption from the support does not play a role. Energy barriers for HCOO formation, relative to direct dissociation barriers of CO₂, indicate that a hydrogen-assisted reduction path is more likely to occur on Cu/WC(0001) materials, with Cu_ML/metallic termination being the most active system for this reaction path. On the other hand, CO₂ adsorption on Cu_ML surfaces is slightly weaker on a C-terminated surface than on a metal-terminated surface, although both surfaces have similar dissociation barriers. This fact together with the weaker CO adsorption on Cu_ML/C-terminated WC(0001) than on metal-terminated WC(0001) suggests that the former system may be a better catalyst for CO₂ reduction, due to the lower surface poisoning by the CO₂ dissociation products. Possible deactivation of Cu/WC(0001) materials may be prevented by the introduction of hydrogen into the system, thus promoting the formation of HCOO and avoiding CO and O formation.

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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:: 1642410

Alternate ID(s):: OSTI ID: 1632973

Report Number(s):: BNL-216187-2020-JAAM

Journal Information:: Physical Chemistry Chemical Physics. PCCP (Print), Vol. 22, Issue 24; ISSN 1463-9076

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 14 works

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