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Morphology and crystal-plane effects of Zr-doped CeO2 nanocrystals on the epoxidation of styrene with tert-butylhydroperoxide as the oxidant

Morphology and crystal-plane effects of Zr-doped CeO_2 nanocrystals on the epoxidation of styrene with tert-butylhydroperoxide as the oxidant

作     者:Jia Ren Xin Liu Ruihua Gao Wei-Lin Dai 

作者机构:Department of Chemistry&Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialFudan UniversityShanghai 200433China State Key Laboratory of Molecular Engineering of PolymersDepartment of Macromolecular ScienceFudan UniversityShanghai 200433China 

出 版 物:《Journal of Energy Chemistry》 (能源化学(英文版))

年 卷 期:2017年第26卷第4期

页      面:681-687页

核心收录:

学科分类:081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 

基  金:the financial support from NNSFC(Project 21373054,21303023,21173052) the Natural Science Foundation of Shanghai Science and Technology Committee(08DZ2270500) 

主  题:Morphology effect Zr-doped CeO2 Styrene Selective oxidation Oxygen vacancies 

摘      要:The morphology effect of Zr-doped CeOwas studied in terms of their activities in the selective oxidation of styrene to styrene oxide using tert-butyl hydroperoxide as the oxidant. In the present work, Zrdoped CeOnanorods exhibited the highest catalytic performance(yield of styrene oxide and TOF value)followed by nanoparticles and nanocubes. For the Zr-doped CeOnanorods, the apparent activation energy is 56.3 k J/mol, which is much lower than the values of catalysts supported on nanoparticles and nanocubes(73.3 and 93.4 k J/mol). The high resolution transmission electron microscopy results indicated that(100) and(110) crystal planes are predominantly exposed for Zr-doped CeOnanorods while(100)and(111) for nanocubes,(111) for nanoparticles. The remarkably increased catalytic activity of the Zrdoped CeOnanorods is mainly attributed to the higher percentage of Cespecies and more oxygen vacancies, which are associated with their exposed(100) and(110) crystal planes. Furthermore, recycling studies proved that the heterogeneous Zr-doped CeOnanorods did not lose its initial high catalytic activity after five successive recycles.

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