Pd/CeO2催化CO氧化活性对载体CeO2形貌的依赖效应

doi:10.7523/j.issn.2095-6134.2015.05.004

摘要/Abstract

摘要：

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.

关键词: Pd/CeO₂界面, 形貌依赖, CO 氧化, 纳米立方块, 纳米八面体

Abstract:

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 PdO_x 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

中图分类号:

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.

WANG Lei, MAO Junyi, YUAN Qing, HUANG Tao. Shape-dependent effects of nanoceria on the activity of Pd/CeO₂ catalysts for CO oxidation[J]. , 2015, 32(5): 594-604.

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Pd/CeO₂催化CO氧化活性对载体CeO₂形貌的依赖效应

Shape-dependent effects of nanoceria on the activity of Pd/CeO₂ catalysts for CO oxidation

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