On the dynamics and reversibility of the deactivation of a Rh/CeO2ZrO2 catalyst in raw bio-oil steam reforming |
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| Affiliation: | 1. Department of Chemical Engineering, University of the Basque Country (UPV/EHU), P.O. Box 644-48080, Bilbao, Spain;2. Department of Chemical and Metallurgical Engineering, School of Chemical Engineering, Aalto University, Espoo, 02150, Finland;1. Department of Mechanical Engineering, University College London, London, WC1E 7JE, UK;2. State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou, 310027, China;1. School of Chemical Engineering, Xiangtan University, Xiangtan, Hunan, 411105, PR China;2. National & Local United Engineering Research Centre for Chemical Process Simulation and Intensification, Xiangtan University, Xiangtan, Hunan, 411105, PR China;1. Environmental and Chemical Engineering, Faculty of Technology, University of Oulu, POB 4300, FI-90014 University of Oulu, Finland;2. Department of Materials Science, Tampere University of Technology, POB 589, FI-33101 Tampere, Finland;3. Department of Applied Physics, Aalto University, POB 15100, FI-00076 Aalto, Finland;4. Dinex Ecocat Oy, POB 20, Vihtavuorentie 162, FI-41331 Vihtavuori, Finland;1. UNILAB, State Key Lab of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai 200237, PR China;2. Shanghai Key Laboratory of Green Chemistry and Chemical Processes, Department of Chemistry, East China Normal University, Shanghai 200062, PR China;3. Instrumental Analysis Center, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, PR China |
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| Abstract: | The deactivation mechanism of a commercial Rh/CeO2 ZrO2 catalyst in raw bio-oil steam reforming has been studied by relating the evolution with time on stream of the bio-oil conversion and products yields and the physicochemical properties of the deactivated catalyst studied by XRD, TPR, SEM, XPS, TPO and TEM. Moreover, the reversibility of the different deactivation causes has been assessed by comparing the behavior and properties of the catalyst fresh and regenerated (by coke combustion with air). The reactions were carried out in an experimental device with two units in series: a thermal treatment unit (at 500 °C, for separation of pyrolytic lignin) and a fluidized bed reactor (at 700 °C, for the reforming reaction). The results evidence that structural changes (support aging involving partial occlusion of Rh species) are irreversible and occur rapidly, being responsible for a first deactivation period, whereas encapsulating coke deposition (with oxygenates as precursors) is reversible and evolves more slowly, thus being the main cause of the second deactivation period. The deactivation selectively affects the reforming of oxygenates, from least to greatest reactivity. Rh sintering is not a significant deactivation cause at the studied temperature. |
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| Keywords: | Bio-oil Hydrogen Steam reforming Rh catalyst Deactivation |
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