| Autor: |
Robert Gleißner, Simon Chung, Guilherme D. L. Semione, Leon Jacobse, Michael Wagstaffe, Steffen Tober, A. Joanne Neumann, Gökhan Gizer, Christopher M. Goodwin, Markus Soldemo, Mikhail Shipilin, Patrick Lömker, Christoph Schlueter, Olof Gutowski, Matthias Muntwiler, Peter Amann, Heshmat Noei, Vedran Vonk, Andreas Stierle |
| Rok vydání: |
2022 |
| Popis: |
We investigated Cu/ZnO model catalysts for methanol synthesis to obtain an atomistic picture of activation and deactivation processes under in situ oxidizing and reducing conditions. We have investigated Cu nanoparticles with different shapes and aspect ratios grown epitaxially on basal and vicinal ZnO surfaces at elevated gas pressures by high energy grazing incidence X-ray diffraction and ambient pressure X-ray photoelectron spectroscopy (AP-XPS). We find that the Cu nanoparticles are fully oxidized to Cu2O under atmospheric conditions at room temperature. During oxidation, they maintain their epitaxy on basal ZnO (000-1) surfaces, whereas on the vicinal ZnO (10-14) surface, the nanoparticles undergo a coherent tilt. We find that the oxidation process is fully reversible under H2 flow at 500 K, resulting in predominantly well-aligned nanoparticles on the basal surfaces, whereas a random orientation is preferred for the (10-14) surface. Under CO2 flow, no diffraction signal from the nanoparticles is detected, pointing to their completely disordered state. The AP-XPS results are in line with the formation of CuO. The analysis of the substrate crystal truncation rods evidences the stability of basal ZnO surfaces under all gas conditions. No proof for Cu-Zn alloy formation is found. Scanning electron microscopy images show that massive mass transport has set in, leading to the formation of larger agglomerates, which is detrimental to the catalyst’s performance. |
| Databáze: |
OpenAIRE |
| Externí odkaz: |
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