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Unravelling the Role of Oxygen Vacancies in the Mechanism of the Reverse Water–Gas Shift Reaction by Operando DRIFTS and Ultraviolet–Visible Spectroscopy
Open accessAbstract
The reaction mechanism of the reverse water–gas shift (RWGS) reaction was investigated using two commercial gold-based catalysts supported on Al 2 O 3 and TiO 2 . 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/Al 2 O 3 proceeds through the formation of formate intermediates that are reduced to CO. In the case of the Au/TiO 2 catalyst, the reaction goes through a redox mechanism with the suggested formation of hydroxycarbonyl intermediates, which further decompose to CO and water. The Ti 3+ 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 CO 2 on Au particles can be discarded. To complete the study, operando ultraviolet–visible spectroscopy was successfully applied to confirm the presence of Ti 3+ and to understand the role of the oxygen vacancies of TiO 2 support in activating CO 2 and thus the subsequent RWGS reaction.
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Metadata
- Authors
- Bobadilla, L. F., Santos, J. L., Ivanova, S., Odriozola, J. A., & Urakawa, A.
- Venue
- ACS Catalysis
- Publisher
- American Chemical Society (ACS)
- Published
- 2018-07-03
- Volume
- 8
- Issue
- 8
- Pages
- 7455-7467
- ISSN
- 2155-5435 (ISSN-L)
- OpenAlex
- W2811097118
- Cited by
- 375
- References
- 29
- FWCI
- 5.24
- Type
- journal article
- Language
- en
- Open access
- green
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