Pulse-response TAP studies of the reverse water–gas shift reaction over a Pt/CeO2 catalyst |
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| Affiliation: | 1. CenTACat, School of Chemistry and Chemical Engineering, Queen''s University Belfast, Belfast BT9 5AG, Northern Ireland, UK;2. Washington University, Department of Chemical Engineering, St Louis, MO 63130, USA;1. Department of Chemical and Process Engineering, University of Surrey, Guildford, GU2 7XH, United Kingdom;2. Laboratorio de Materiales Avanzados, Departamento de Química Inorgánica Instituto Universitario de Materiales de Alicante Universidad de Alicante, Apartado 99, E-03080 Alicante, Spain;1. Petroleum University of Technology, Ahwaz Faculty of Petroleum Engineering, Chemical Engineering Department, Ahwaz, Iran;2. Petroleum University of Technology, Ahwaz Faculty of Petroleum Engineering, Science Department, Ahwaz, Iran;1. Departament de Química Inorgànica i Orgànica, Secció de Química Inorgànica and Institut de Nanociència i Nanotecnologia (IN2UB), Universitat de Barcelona, Martí i Franquès 1-11, 08028 Barcelona, Spain;2. Catalonia Institute for Energy Research (IREC), Jardins de les Dones de Negre 1, 08930 Barcelona, Spain;3. Departament de Ciència de Materials i Química Física & Institut de Química Teòrica i Computacional (IQTCUB), Universitat de Barcelona, Martí i Franquès 1-11, 08028 Barcelona, Spain;4. École Nationale Supérieure des Ingénieurs en Arts Chimiques et Technologiques (INP-ENSIACET), 4 Allée Emile Monso, 31030 Toulouse, France;1. Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, School of Environment and Energy, South China University of Technology, Guangzhou 510006, China;2. National Engineering Laboratory for VOCs Pollution Control Technology and Equipment, South China University of Technology, Guangzhou 510006, China |
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| Abstract: | The temporal analysis of products (TAP) technique was successfully applied for the first time to investigate the reverse water–gas shift (RWGS) reaction over a 2% Pt/CeO2 catalyst. The adsorption/desorption rate constants for CO2 and H2 were determined in separate TAP pulse-response experiments, and the number of H-containing exchangeable species was determined using D2 multipulse TAP experiments. This number is similar to the amount of active sites observed in previous SSITKA experiments. The CO production in the RWGS reaction was studied in a TAP experiment using separate (sequential) and simultaneous pulsing of CO2 and H2. A small yield of CO was observed when CO2 was pulsed alone over the reduced catalyst, whereas a much higher CO yield was observed when CO2 and H2 were pulsed consecutively. The maximum CO yield was observed when the CO2 pulse was followed by a H2 pulse with only a short (1 s) delay. Based on these findings, we conclude that an associative reaction mechanism dominates the RWGS reaction under these experimental conditions. The rate constants for several elementary steps can be determined from the TAP data. In addition, using a difference in the time scale of the separate reaction steps identified in the TAP experiments, it is possible to distinguish a number of possible reaction pathways. |
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