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Synergistic Catalysis of Carbon Monoxide Oxidation over Copper Oxide Supported on Samaria-Doped Ceria

机译:掺杂Samaria的氧化铈负载氧化铜对一氧化碳的协同催化作用

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Copper oxide supported on samaria-doped ceria (SDC) is chosen as a model catalyst for carbon as a model catalyst for carbon monoxide oxidation to illustrate interfacial metal oxide-support interaction and synergism. The oxidation catalysis by CuO/SDC was studied to further elucidate the effect of oxygen vacancies on activity enhancement and light-off behavior. It was found that an approximate proportionality exists between the reducibility and the activity of catalysts. It is concluded that reducibility and susceptibility of change of oxidation states of coper oxides is key to catalytic activities, and the nonstoichiometric metastable copper oxide species formed during reduction are very active because of their superior capability to transport surface lattice oxygen. A preliminary mechanism involving surface lattice oxygen of CuO and oxygen vacancy participation is proposed to fully explicate the synergistic process leading to light-off. The cause of light-off is attributed to the formation of co-shared oxyen sites which are composed to metastable copper oxide species and oxyen vacancies of two types, V_(o, CuO) and V_(o, SDC). Over these CuO/SDC catalysts, the active sites exhibit the Langmuir-Hinshelwood-type mechanism characteristic of precious metals although the redox-cycle mechanism still operative.
机译:选择负载在掺​​杂samaria的二氧化铈(SDC)上的氧化铜作为碳的模型催化剂,作为一氧化碳氧化的模型催化剂,以说明界面金属氧化物与载体的相互作用和协同作用。研究了CuO / SDC的氧化催化作用,以进一步阐明氧空位对活性增强和起燃行为的影响。发现在催化剂的还原性和活性之间存在近似比例。结论是铜氧化物的氧化态变化的还原性和敏感性是催化活性的关键,并且还原过程中形成的非化学计量的亚稳态氧化铜由于其表面氧的传递能力强而非常活跃。提出了涉及CuO的表面晶格氧和氧空位参与的初步机理,以充分阐明导致起燃的协同过程。起火的原因归因于形成共共享的氧位点,该位点由亚稳态的氧化铜种类和两种类型的氧空位(V_(o,CuO)和V_(o,SDC))组成。在这些CuO / SDC催化剂上,尽管氧化还原循环机理仍然有效,但活性部位仍具有贵金属的Langmuir-Hinshelwood型机理。

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