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In situ DRIFT spectroscopy insights into the reaction mechanism of CO and toluene co-oxidation over Pt-based catalysts

机译:原位光谱漂移的见解公司和甲苯共氧化反应机制在Pt-based催化剂

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摘要

Considering that the mutual inhibition between CO and hydrocarbon (HC) co-oxidation over platinumgroup metal (PGM) catalysts is a universal problem, in this study, a series of Pt-supported catalysts (Pt-Al2O3, Pt-Co3O4 and Pt-CeO2) were synthesized by combining glycol reduction and electrostatic chemical adsorption, and then were evaluated for the catalytic oxidation of CO and toluene. The Pt-CeO2 catalyst exhibited the best catalytic performance for individual CO and toluene oxidation, and effectively slowed down the competitive reaction in the presence of both CO and toluene. This superior performance over the Pt-CeO2 catalyst was associated with the formation of strong metal-support interactions (SMSIs) between the surface oxygen and adjacent Pt species. The formation of SMSIs not only enhanced the activation and migration of oxygen species and the formation of surface oxygen vacancies, but also improved the lower temperature reducibility of the catalyst. The in situ DRIFTS spectra revealed that CO was first transformed into carbon-related species (bicarbonates and carbonates), and then completely decomposed into CO2. Moreover, the reaction route for toluene oxidation may follow only one successive step: benzyl radical -> benzaldehyde -> benzoate -> formate species, and finally completely oxidized to CO2 and H2O. The reaction pathways between CO and toluene oxidation may be independent when CO and toluene co-exist, although their reaction rates slow down due to the competitive adsorption between CO and toluene molecules at the same sites.
机译:考虑到公司之间的相互抑制和碳氢化合物(HC)共氧化platinumgroup金属(PGM)是一种催化剂普遍问题,在这项研究中,一个系列的Pt-supported催化剂(Pt-Al2O3 Pt-Co3O4和Pt-CeO2)被结合醇合成减少和静电化学吸附,然后进行催化CO和甲苯的氧化。表现出最好的催化性能个人公司和甲苯氧化有效地减缓竞争反应在公司和甲苯的存在。Pt-CeO2催化剂性能优越与强大的形成金属支架(SMSIs)之间的交互表面氧和相邻Pt的物种。形成SMSIs不仅提高了激活和氧物种和迁移表面氧空位的形成,但是也提高了低温度还原性的催化剂。透露,公司最初转化成(重碳酸盐和carbon-related物种碳酸盐),然后完全分解成二氧化碳。氧化可能仅遵循一个连续的步骤:苄激进- >苯甲醛-苯甲酸> >甲酸的物种,最后完全氧化二氧化碳和水。和甲苯氧化可能独立时有限公司和甲苯共存,尽管他们的反应利率降低由于竞争吸附有限公司和甲苯分子之间是一样的网站。

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