Journal
ACS CATALYSIS
Volume 8, Issue 8, Pages 7455-7467Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.8b02121
Keywords
RWGS; Au-based catalysts; operando; DRIFTS; UV-vis
Categories
Funding
- Spanish Ministerio de Economia y Competitividad (MINECO) [ENE2013-47880-C3-2-R, ENE2015-66975-C3-2-R]
- MINECO
- Generalitat de Catalunya through the CERCA Programme and recognition [2014 SGR 893]
- MINECO (AEI/FEDER-UE) [CTQ2016-75499-R]
- Severo Ochoa Excellence Accreditation 2014-2018 [SEV-2013-0319]
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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 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 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.
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