Effect of Different In2 O3 (111) Surface Terminations on CO2 Adsorption
Journal article, 2023
In2O3-based catalysts have shown high activity and selectivity for CO2 hydrogenation to methanol; however, the origin of the high performance of In2O3 is still unclear. To elucidate the initial steps of CO2 hydrogenation over In2O3, we have combined X-ray photoelectron spectroscopy and density functional theory calculations to study the adsorption of CO2 on the In2O3(111) crystalline surface with different terminations, namely, the stoichiometric, reduced, and hydroxylated surface. The combined approach confirms that the reduction of the surface results in the formation of In adatoms and that water dissociates on the surface at room temperature. A comparison of the experimental spectra and the computed core-level shifts (using methanol and formic acid as benchmark molecules) suggests that CO2 adsorbs as a carbonate on all three surface terminations. We find that the adsorption of CO2 is hindered by hydroxyl groups on the hydroxylated surface.
indium oxide
density functional theory
core-level shifts
methanol synthesis
heterogeneous catalysis
X-ray photoelectron spectroscopy
CO2 adsorption
Author
Sabrina M. Gericke
Lund University
Minttu Maria Kauppinen
Chalmers, Physics, Chemical Physics
Margareta Wagner
Vienna University of Technology
Michele Riva
Vienna University of Technology
Giada Franceschi
Vienna University of Technology
Alvaro Posada Borbon
Chalmers, Physics, Chemical Physics
Lisa Rämisch
Lund University
Sebastian Pfaff
Lund University
Erik Rheinfrank
Vienna University of Technology
Alexander M. Imre
Vienna University of Technology
Alexei B. Preobrajenski
MAX IV Laboratory
Stephan Appelfeller
MAX IV Laboratory
Sara Blomberg
Institutionen för Kemiteknik
L. R. Merte
Malmö university
Johan Zetterberg
Lund University
Ulrike Diebold
Vienna University of Technology
Henrik Grönbeck
Chalmers, Physics, Chemical Physics
Edvin Lundgren
Lund University
ACS Applied Materials & Interfaces
1944-8244 (ISSN) 1944-8252 (eISSN)
Vol. 15 38 45367-45377Adaptive multiscale modeling in heterogeneous catalysis
Swedish Research Council (VR) (2020-05191), 2021-01-01 -- 2024-12-31.
Atomistic Design of Catalysts
Knut and Alice Wallenberg Foundation (KAW2015.0058), 2016-01-07 -- 2021-06-30.
Subject Categories
Physical Chemistry
Theoretical Chemistry
DOI
10.1021/acsami.3c07166
PubMed
37704018