金属核及氧化铈的物理化学性质对一氧化碳氧化的影响

doi:10.1016/S1872-2067(20)63557-4

摘要/Abstract

摘要： 氧化铈独特的氧化还原性能使其适合用作氧化反应中的催化剂或载体.氧化铈负载的过渡金属纳米粒子或孤立的单原子提供了金属-载体界面，从而降低了去除界面氧原子的能耗，提供了可以参与Man Van Kulvian氧化过程的活性氧物种.CO氧化是测试氧化铈负载催化剂还原性的主要探针反应，并且它常见于在相对低温下消除CO的各种应用中.在过量H₂中优先氧化CO（PROX）反应可控制CO浓度达到超低水平，以防止氢氧化电催化剂中毒.催化剂在CO氧化反应中的活性和在PROX反应中对CO和H₂的选择性取决于金属物种的种类和分散性、CeO₂的结构和化学性质以及催化剂的合成方法.在这篇综述中，我们总结了最近发表的关于CeO₂负载的金属纳米粒子和单原子催化CO氧化和PROX反应的相关工作；以及不同的负载金属和同种金属在普通CeO₂表面上的反应性.我们还总结了密度泛函理论计算中提出的最可能的反应机理；并且讨论了各种负载型金属在PROX反应中影响CO氧化选择性的因素.

关键词: 氧化铈, CO氧化, 金属纳米粒子, 单原子, PROX

Abstract: The redox properties of ceria make it suitable as a catalyst or support in oxidation reactions. Ceria-supported transition metal nanoparticles or isolated single atoms provide a metal-support interface that reduces the energy cost to remove interfacial oxygen atoms, providing active oxygen species that can participate in Mars van Krevelen oxidation processes. CO oxidation is a key probe reaction to test the reducibility of ceria-supported catalysts and is also practically important in the elimination of CO at relatively low temperatures in various applications. Preferential oxidation of CO (PROX) in excess H₂ controls the CO concentration to ultra-low levels to prevent poisoning of hydrogen oxidation electrocatalysts. The reactivity of catalysts in CO oxidation and selectivity towards CO over H₂ in PROX is dependent on the type and dispersion of metal species, the structural and chemical properties of CeO₂, and the synthetic preparation methods of the catalysts. In this review, we summarize recently published works on catalytic CO oxidation and PROX reactions on ceria-supported metal nanoparticles and single atoms. We summarize the reactivity on different supported metals, and on different CeO₂ surfaces with the same metal. We summarize the most likely reaction mechanisms as suggested by density functional theory calculations. The factors contributing to selectivity towards CO oxidation in PROX reactions on various supported metals are also discussed.

Key words: Ceria, CO oxidation, Metal nanoparticles, Single atoms, Preferential oxidation of CO, Metal nuclearity

Linxi Wang, Shyam Deo, Kerry Dooley, Michael J. Janik, Robert M. Rioux. 金属核及氧化铈的物理化学性质对一氧化碳氧化的影响[J]. 催化学报, 2020, 41(6): 951-962.

Linxi Wang, Shyam Deo, Kerry Dooley, Michael J. Janik, Robert M. Rioux. Influence of metal nuclearity and physicochemical properties of ceria on the oxidation of carbon monoxide[J]. Chinese Journal of Catalysis, 2020, 41(6): 951-962.

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