The effect of sulfur dioxide on the activity of hierarchical Pd-based catalysts in methane combustion
المؤلف | Monai, Matteo |
المؤلف | Montini, Tiziano |
المؤلف | Melchionna, Michele |
المؤلف | Duchon, Tomas |
المؤلف | Kus, Peter |
المؤلف | Chen, Chen |
المؤلف | Tsud, Nataliya |
المؤلف | Nasi, Lucia |
المؤلف | Prince, Kevin C. |
المؤلف | Veltruska, Katerina |
المؤلف | Matolin, Vladimir |
المؤلف | Khader, Mahmoud M. |
المؤلف | Gorte, Raymond J. |
المؤلف | Fornasiero, Paolo |
تاريخ الإتاحة | 2021-02-08T09:14:52Z |
تاريخ النشر | 2017 |
اسم المنشور | Applied Catalysis B: Environmental |
المصدر | Scopus |
الملخص | SO2 poisoning of methane oxidation over alumina-supported, Pd@CexZr1−xO2 nanoparticle catalysts was systematically studied by means of advanced PhotoElectron Spectroscopy (PES) methods. The Pd@CexZr1−xO2 units were synthesized and deposited on two modified-alumina supports, i.e. high surface area modified alumina and a model alumina prepared by Atomic Layer Deposition (ALD) of alumina on Indium Tin Oxide (ITO)/quartz slides. The model support was designed to be suitable for PES analysis and was stable to high temperature treatments (850 °C). Characterization of the high-surface-area (HSA) catalysts by X-Ray Diffraction (XRD), N2 physisorption, CO chemisorption and Transmission Electron Microscopy (TEM) indicated formation of CeO2–ZrO2 (CZ) mixed-oxide crystallites that stabilize the Pd active phase against sintering. Correlation of methane-oxidation rates with PES results demonstrated two distinct mechanisms for deactivation by SO2. Below 450 °C, the presence of SO2 in the feed led to partial reduction of the active PdO phase and to the formation of sulfates on the Pd. Above 500 °C, poisoning by SO2 was less severe due to spillover of the sulfates onto the oxide promoter. Pd@ZrO2 catalysts showed the best resistance to SO2 poisoning, outperforming analogous Pd@CZ mixed-oxide catalysts, because there was less sulfate formation and the sulfates that did form could be removed during regeneration. |
راعي المشروع | The authors acknowledge CERIC-ERIC for open access to instrumentation and user support. This paper was also made possible by a NPRP Grant #6-290-1-059 from the Qatar National Research Fund (a member of Qatar Foundation). The statements made herein are solely the responsibility of the authors. |
اللغة | en |
الناشر | Elsevier B.V. |
الموضوع | Ceria-Zirconia Methane oxidation catalysts Palladium Sulfur dioxide XPS |
النوع | Article |
الصفحات | 72-83 |
رقم المجلد | 202 |
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