| Title: |
The influence of size, metal loading and oxygen vacancies on the catalytic performance of Au/ CeO2−x in the sunlight-powered reverse water gas shift reaction |
| Authors: |
Volders, Jordi; Bossier, Sander; Stulens, Sande; Joos, Bjorn; Vranken, T.; Sastre, Francesc; D'Haen, Jan; Elen, Ken; Verheijen, Marcel A.; Cool, Pegie; Hardy, An; Buskens, Pascal J.P.; van Bael, Marlies K. |
| Source: |
Volders, J, Bossier, S, Stulens, S, Joos, B, Vranken, T, Sastre, F, D'Haen, J, Elen, K, Verheijen, M A, Cool, P, Hardy, A, Buskens, P J P & van Bael, M K 2025, 'The influence of size, metal loading and oxygen vacancies on the catalytic performance of Au/ CeO2−x in the sunlight-powered reverse water gas shift reaction', Catalysis Science & Technology, vol. 15, no. 2, pp. 486-500. https://doi.org/10.1039/d4cy01194e |
| Publication Year: |
2025 |
| Description: |
This study reports the conversion of CO2 and H2 to CO and H2O at low temperature and low pressure (up to 203 °C, p = 3.5 bar) using plasmonic Au/CeO2−x photocatalysts, with mildly concentrated sunlight as the sole energy source (up to 9 kW m−2). Systematic catalytic studies were carried out by varying the CeO2−x particle size, Au particle size and loading, and the concentration of oxygen vacancies. Upon illumination, all Au/CeO2−x catalysts showed a CO production of up to 2.6 ± 0.2 mmol CO per gAu per h (104 ± 8 μmol CO per gcat per h), while the supports without Au did not show any activity. We determined that both photothermal and non-thermal effects contribute to the light-driven reverse water-gas shift reaction catalysed by plasmonic Au/CeO2−x. A photothermal contribution was found from the exponential relationship between the CO production and the solar irradiance. In the dark, all Au/CeO2−x photocatalysts and supports without Au produced CH4 instead of CO with ≥97% selectivity, indicating a significant non-thermal contribution in light. A linear dependence of catalytic activity on the accessible interface area between CeO2−x and Au was found, which is in line with an associative formate-mediated reaction mechanism occurring at the metal–support interface. Tuning the VO content through thermal treatments yielded decreased photocatalytic activity for oxidised samples, identifying them as pre-catalysts. The stability of the Au/CeO2−x photocatalysts was evaluated, demonstrating that the catalytic performance was affected by adsorption of H2O as a reaction product, which could be fully restored upon heating in vacuo. |
| Document Type: |
article in journal/newspaper |
| File Description: |
application/pdf |
| Language: |
English |
| ISSN: |
2044-4753; 2044-4761 |
| Relation: |
info:eu-repo/semantics/altIdentifier/pissn/2044-4753; info:eu-repo/semantics/altIdentifier/eissn/2044-4761 |
| DOI: |
10.1039/d4cy01194e |
| Availability: |
https://research.tue.nl/en/publications/569573da-8c75-4a59-a664-b7e1bd2d19ff; https://doi.org/10.1039/d4cy01194e; https://pure.tue.nl/ws/files/351492742/d4cy01194e.pdf; https://www.scopus.com/pages/publications/85212263157 |
| Rights: |
info:eu-repo/semantics/openAccess ; http://creativecommons.org/licenses/by-nc/4.0/ |
| Accession Number: |
edsbas.94EB6AD0 |
| Database: |
BASE |