A1 Journal article (refereed)
Influence of a Cu–zirconia interface structure on CO2 adsorption and activation (2021)

Gell, L., Lempelto, A., Kiljunen, T., & Honkala, K. (2021). Influence of a Cu–zirconia interface structure on CO2 adsorption and activation. Journal of Chemical Physics, 154, Article 214707. https://doi.org/10.1063/5.0049293

JYU authors or editors

Gell, Lars
Lempelto, Aku
Kiljunen, Toni
Honkala, Karoliina

Publication details

All authors or editors: Gell, Lars; Lempelto, Aku; Kiljunen, Toni; Honkala, Karoliina

Journal or series: Journal of Chemical Physics

ISSN: 0021-9606

eISSN: 1089-7690

Publication year: 2021

Publication date: 07/06/2021

Volume: 154

Article number: 214707

Publisher: American Institute of Physics

Publication country: United States

Publication language: English

DOI: https://doi.org/10.1063/5.0049293

Publication open access: Not open

Publication channel open access:

Publication is parallel published (JYX): https://jyx.jyu.fi/handle/123456789/80353

Web address of parallel published publication (pre-print): https://chemrxiv.org/articles/preprint/Influence_of_a_Cu-Zirconia_Interface_Structure_on_CO2_Adsorption_and_Activation/14176523/1

Abstract

CO2 adsorption and activation on a catalyst are key elementary steps for CO2 conversion to various valuable products. In the present computational study, we screened different Cu–ZrO2 interface structures and analyzed the influence of the interface structure on CO2 binding strength using density functional theory calculations. Our results demonstrate that a Cu nanorod favors one position on both tetragonal and monoclinic ZrO2 surfaces, where the bottom Cu atoms are placed close to the lattice oxygens. In agreement with previous calculations, we find that CO2 prefers a bent bidentate configuration at the Cu–ZrO2 interface and the molecule is clearly activated being negatively charged. Straining of the Cu nanorod influences CO2 adsorption energy but does not change the preferred nanorod position on zirconia. Altogether, our results highlight that CO2 adsorption and activation depend sensitively on the chemical composition and atomic structure of the interface used in the calculations. This structure sensitivity may potentially impact further catalytic steps and the overall computed reactivity profile.

Keywords: carbon dioxide; carbon capture and storage; adsorption; catalysts; nanoparticles; copper; zirconium dioxide; thermodynamics; density functional theory