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Transient behavior and reaction mechanism of CO catalytic ignition over a CuO-CeO 2 mixed oxide
Kang,Running1,2; Ma,Pandong1,3; He,Junyao1; Li,Huixin1; Bin,Feng1,2,4; Wei,Xiaolin1,2,4; Dou,Baojuan3; Hui,Kwun Nam5; Hui,Kwan San6
2021-01
Source PublicationProceedings of the Combustion Institute
ISSN1540-7489
Abstract

This study focuses on the variation in activity-controlling factors during CO catalytic ignition over a CuO–CeO2 catalyst. The activity for CO combustion follows the decreasing order of CuO–CeO2 > CuO > CeO2. Except for inactive CeO2, increasing temperature induces CO ignition to achieve self-sustained combustion over CuO and CuO–CeO2. However, CuO provides enough copper sites to adsorb CO, and abundant active lattice oxygen, thus obtaining a higher hot zone temperature (208.3°C) than that of CuO–CeO2 (197.3 °C). Catalytic ignition triggers a kinetic transition from the low-rate steady-state regime to a high-rate steady-state regime. During the induction process, Raman, X-ray photoelectron spectroscopy (XPS), CO temperature-programmed desorption (CO-TPD) and infrared (IR) spectroscopy results suggested that CO is preferentially adsorbed on oxygen vacancies (Cu+-[Ov]-Ce3+) to yield Cu+-[Ctriple bondO]-Ce3+ complexes. Because of the self-poisoning of CO, the adsorbed CO and traces of adsorbed oxygen react at a relative rate, which is entirely governed by the kinetics on the CO-covered surface and the heat transport until the pre-ignition regime. Nonetheless, the Cu+-[Ctriple bondO]-Ce3+ complex is a major contributor to CO ignition. The step-response runs and kinetic models testified that after ignition, a kinetic phase transition occurs from a CO-covered surface to an active lattice oxygen-covered surface. During CO self-sustained combustion, the rapid gas diffusivity and mass transfer is beneficial for handling the low coverage of CO. The active lattice oxygen of CuO takes part in CO oxidation.

KeywordCarbon Monoxide Catalytic Ignition Copper-cerium Oxide Reaction Mechanism Transient Behavior
DOI10.1016/j.proci.2020.06.186
URLView the original
Indexed BySCIE
Language英語English
WOS Research AreaThermodynamics ; Energy & Fuels ; Engineering
WOS SubjectThermodynamics ; Energy & Fuels ; Engineering, Chemical ; Engineering, Mechanical
WOS IDWOS:000640405500004
PublisherELSEVIER SCIENCE INC, STE 800, 230 PARK AVE, NEW YORK, NY 10169 USA
Scopus ID2-s2.0-85090444676
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Cited Times [WOS]:8   [WOS Record]     [Related Records in WOS]
Document TypeJournal article
CollectionINSTITUTE OF APPLIED PHYSICS AND MATERIALS ENGINEERING
Corresponding AuthorBin,Feng; Hui,Kwan San
Affiliation1.State Key Laboratory of High-Temperature Gas Dynamics, Institute of Mechanics, Chinese Academy of Sciences, Beijing 100190, PR China
2.School of Engineering Science, University of Chinese Academy of Sciences, 100049 Beijing, PR China
3.Tianjin University of Science & Technology, Tianjin 300457, PR China
4.Dalian National Laboratory for Clean Energy, Dalian 116023, PR China
5.Institute of Applied Physics and Materials Engineering, University of Macau, Avenida da Universidade, Taipa, Macau, PR China
6.Engineering, Faculty of Science, University of East Anglia, Norwich Research Park, NR4 7TJ, United Kingdom
Recommended Citation
GB/T 7714
Kang,Running,Ma,Pandong,He,Junyao,et al. Transient behavior and reaction mechanism of CO catalytic ignition over a CuO-CeO 2 mixed oxide[J]. Proceedings of the Combustion Institute,2021.
APA Kang,Running,Ma,Pandong,He,Junyao,Li,Huixin,Bin,Feng,Wei,Xiaolin,Dou,Baojuan,Hui,Kwun Nam,&Hui,Kwan San.(2021).Transient behavior and reaction mechanism of CO catalytic ignition over a CuO-CeO 2 mixed oxide.Proceedings of the Combustion Institute.
MLA Kang,Running,et al."Transient behavior and reaction mechanism of CO catalytic ignition over a CuO-CeO 2 mixed oxide".Proceedings of the Combustion Institute (2021).
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