Shape-dependent effects of nanoceria on the activity of Pd/CeO2 catalysts for CO oxidation
Received date: 2015-04-13
Revised date: 2015-06-15
Online published: 2015-09-15
Pd纳米颗粒的氧化还原性能对Pd/CeO2催化氧化反应的性能至关重要,且与Pd-CeO2的界面结构密切相关.我们发现Pd/CeO2的低温催化CO氧化活性高度依赖于载体CeO2的形貌和暴露晶面.利用胶体沉积法,得到Pd/CeO2八面体和Pd/CeO2立方块两种催化剂.结果表明暴露{111}晶面的CeO2八面体负载Pd催化剂的催化CO氧化活性远优于暴露{100}晶面的CeO2立方块负载Pd催化剂.DFT理论模拟计算结果表明,催化剂表面的Pd物种的氧化还原活性可能决定催化剂的可还原性和催化活性:钯从氧化态到金属态的循环更容易在CeO2(111)上进行,而这取决于Pd与载体CeO2之间的相互作用.我们的结果表明,催化剂表面活性Pd物种的氧化还原性能对Pd/CeO2的催化活性至关重要,可以通过调控载体暴露的晶面实现Pd与载体CeO2之间的相互作用,最终实现对催化剂可还原性和催化活性的可控调变.
王雷 , 毛俊义 , 袁清 , 黄涛 . Pd/CeO2催化CO氧化活性对载体CeO2形貌的依赖效应[J]. 中国科学院大学学报, 2015 , 32(5) : 594 -604 . DOI: 10.7523/j.issn.2095-6134.2015.05.004
The redox property of palladium nanoparticles (NPs) is pivotal to CeO2 supported Pd catalysts in oxidation reactions and is closely related to the structure of Pd-CeO2 interface. Herein, we report that low-temperature CO oxidation activity of Pd/CeO2 highly depends on the shape and crystal plane of CeO2 supports. Pd/CeO2 catalysts with CeO2 nanoocthedrons (NOCs) and nanocubes (NCs) as supports were prepared by colloidal-deposition method. Results show that Pd/CeO2 NOCs with ceria {111} facets enclosed exhibited much higher catalytic activity than Pd/CeO2NCs with ceria {100} facets exposed. DFT calculations revealed that the redox property of surface Pd species may play important roles in determining the reducibility and activity of catalysts. The PdOx to Pd cycle is more facile on Pd4@CeO2(111) than on Pd4@CeO2(100), which is dictated by the Pd-ceria interaction in the end. Our results show that the redox property of surface Pd is pivotal to the reducibility and activity of Pd/ceria catalysts, which could be tuned by manipulation of the Pd-CeO2 interaction via tuning the exposed facets of ceria support.
Key words： Pd/CeO2 interface; shape-dependent; CO oxidation; nanocube; nanooctahedron
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