Artículo
Unravelling the Role of Oxygen Vacancies in the Mechanism of the Reverse Water–Gas Shift Reaction by Operando DRIFTS and Ultraviolet–Visible Spectroscopy
Autor/es | Bobadilla Baladrón, Luis Francisco
Santos Muñoz, José Luis Ivanova, Svetlana Odriozola Gordón, José Antonio Urakawa, Atsushi |
Departamento | Universidad de Sevilla. Departamento de Química Inorgánica |
Fecha de publicación | 2018 |
Fecha de depósito | 2022-10-17 |
Publicado en |
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Resumen | 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 ... 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. |
Agencias financiadoras | Ministerio de Economía y Competitividad (MINECO). España Centres de Recerca de Catalunya (CERCA) Agencia Estatal de Investigación. España European Commission (EC). Fondo Europeo de Desarrollo Regional (FEDER) |
Identificador del proyecto | ENE2013-47880-C3-2-R
ENE2015-66975-C3-2-R CERCA 2014 SGR 893 CTQ2016-75499-R |
Cita | Bobadilla Baladrón, L.F., Santos Muñoz, J.L., Ivanova, S., Odriozola Gordón, J.A. y Urakawa, A. (2018). Unravelling the Role of Oxygen Vacancies in the Mechanism of the Reverse Water–Gas Shift Reaction by Operando DRIFTS and Ultraviolet–Visible Spectroscopy. ACS Catalysis, 8 (8), 7455-7467. https://doi.org/doi.org/10.1021/acscatal.8b02121. |
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