4.7 Article

Morphology effects on surface chemical properties and lattice defects of Cu/CeO2 catalysts applied for low-temperature CO oxidation

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SCIENTIFIC REPORTS
卷 9, 期 -, 页码 -

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NATURE PUBLISHING GROUP
DOI: 10.1038/s41598-019-48606-2

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  1. National Natural Science Foundation of China [21507137, 21707145, 51808529]
  2. West Light Foundation of The Chinese Academy of Sciences [2016-B]

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Here, we synthesized a series of Cu/CeO2 catalysts with different morphology and size, including Cu/CeO2 nanospheres (Cu/CeO2-S), Cu/CeO2 nanoparticles (Cu/CeO2-P), Cu/CeO2 nanorods (Cu/CeO2-R) and flower-like Cu/CeO2 microspheres (Cu/CeO2-F) to systematically explore the structure-activity relationship in CO oxidation. Crucially, the effect of morphology, crystal size, Ce4+/Ce3+ species, oxygen vacancies derived from the removal of lattice oxygen (O-latt) species in CeO2 and lattice defect sites on CO activity was revealed through various characterizations. It was clearly discovered that the activity of these catalysts was as follows: Cu/CeO2-R > Cu/CeO2-P > Cu/CeO2-S > Cu/CeO2-F, and the Cu/CeO2-R catalyst preferentially showed the best catalytic performance with a 90% conversion of CO even at 58 degrees C, owned the smaller particles size of CeO2 and CuO, and exhibited the higher concentration of Olatt species and oxygen vacancies. Besides, it is also verified that the Cu/CeO2-F sample exhibited the larger CeO2 crystal size (17.14 nm), which led to the lower Cu dispersion and CO conversion, even at 121 degrees C (T-90). Most importantly, we discovered that the amount of surface lattice defect sites was positively related to the reaction rate of CO. Simultaneously, DFT calculation also demonstrated that the introduced oxygen vacancies in CeO2 could accelerate the oxidation of CO by the alteration of CO adsorption energy. Therefore, the morphology, the crystal size, the content of oxygen vacancies, as well as lattice defects of Cu/CeO2 catalyst might work together for CO oxidation reaction.

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