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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: ();

机构地区: Department of Chemistry & Shanghai Key Laboratory of Molecular Catalysis and Innovative Material,Fudan University

出  处: 《Journal of Energy Chemistry》 2017年第4期681-687,共7页

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. The morphology effect of Zr-doped CeO_2 was 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 CeO_2 nanorods exhibited the highest catalytic performance(yield of styrene oxide and TOF value)followed by nanoparticles and nanocubes. For the Zr-doped CeO_2 nanorods, 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 CeO_2 nanorods while(100)and(111) for nanocubes,(111) for nanoparticles. The remarkably increased catalytic activity of the Zrdoped CeO_2 nanorods is mainly attributed to the higher percentage of Ce^(3+)species and more oxygen vacancies, which are associated with their exposed(100) and(110) crystal planes. Furthermore, recycling studies proved that the heterogeneous Zr-doped CeO_2 nanorods did not lose its initial high catalytic activity after five successive recycles.

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