Unravelling the Role of Oxygen Vacancies in the Mechanism of the Reverse Water-Gas-Shift Reaction by Operando DRIFTS and UV-Vis Spectroscopy
| Autor: | José Luis Alonso Santos, Atsushi Urakawa, L.F. Bobadilla, José Antonio Odriozola, Svetlana Ivanova |
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| Přispěvatelé: | Bobadilla, L. F. [0000-0003-0085-9811], Bobadilla, L. F. |
| Rok vydání: | 2018 |
| Předmět: |
Reaction mechanism
RWGS Chemistry chemistry.chemical_element UV-Vis 02 engineering and technology General Chemistry 010402 general chemistry 021001 nanoscience & nanotechnology Photochemistry 01 natural sciences Redox Oxygen Catalysis Water-gas shift reaction 0104 chemical sciences chemistry.chemical_compound Ultraviolet visible spectroscopy Adsorption DRIFTS Formate Operando 0210 nano-technology Gold-based catalyst |
| Zdroj: | Digital.CSIC. Repositorio Institucional del CSIC instname |
| Popis: | The reaction mechanism of the reverse water–gas shift (RWGS) reaction was investigated using two commercial gold-based catalysts supported on Al2O3 and TiO2. The surface species formed during the reaction and reaction mechanisms were elucidated by transient and steady-state operando DRIFTS studies. It was revealed that RWGS reaction over Au/Al2O3 proceeds through the formation of formate intermediates that are reduced to CO. In the case of the Au/TiO2 catalyst, the reaction goes through a redox mechanism with the suggested formation of hydroxycarbonyl intermediates, which further decompose to CO and water. The Ti3+ species, the surface hydroxyls, and oxygen vacancies jointly participate. The absence of carbonyl species adsorbed on gold particles during the reaction for both catalysts indicates that the reaction pathway involving dissociative adsorption of CO2 on Au particles can be discarded. To complete the study, operando ultraviolet–visible spectroscopy was successfully applied to confirm the presence of Ti3+ and to understand the role of the oxygen vacancies of TiO2 support in activating CO2 and thus the subsequent RWGS reaction. |
| Databáze: | OpenAIRE |
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