Regensburg 2022 – scientific programme
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O: Fachverband Oberflächenphysik
O 62: Surface Reactions and Heterogeneous Catalysis 1
O 62.2: Talk
Thursday, September 8, 2022, 10:45–11:00, H4
Hydrogen adsorption on Pd surfaces and its effect on CO2 activation — •Herzain I. Rivera-Arrieta1, Igor Kowalec2, Lucas Foppa1, Andrew Logsdail2, David Willock2, and Matthias Scheffler1 — 1The NOMAD Laboratory at the Fritz Haber Institute of the Max Planck Society and the Humboldt-Universität zu Berlin, Germany — 2Cardiff Catalysis Institute, Cardiff University, UK
Understanding the reactivity of Pd-based catalysts in hydrogenation processes requires an accurate description of its surfaces at realistic temperature (T) and hydrogen pressure (pH2). Herein, by modeling the surface phase diagram of Pd (111) and (100) as a function of T, pH2 via ab initio atomistic thermodynamics [1], we predict 1 monolayer (ML) coverage of H as the most stable configuration under common experimental reaction conditions [2]. Taking a particular interest in the activation of CO2, we performed simulations concerning the interaction of the molecule with the surfaces as the H-coverage increases from 0 to 1ML. Our results show how 1 ML of H inhibits the formation of chemisorbed CO2δ-, the initial intermediate in the CO2 hydrogenation reaction. The generated data will be combined with information from other metal surfaces, and the subgroup-discovery artificial-intelligence approach [3] will be applied to identify which basic materials parameters correlate with indicators of CO2 activation, e.g. the adsorption energy or the C-O bond elongation.
[1] C. Stampfl, et al., Appl. Phys. A, 69, 471 (1999).
[2] H. Bahruji, et al., J. Catal., 343, 133 (2016).
[3] B. R. Goldsmith, et al., New J. Phys., 19, 013031 (2017).