4.6 Article

Facile preparation of 3D ordered mesoporous CuOx-CeO2 with notably enhanced efficiency for the low temperature oxidation of heteroatom-containing volatile organic compounds

期刊

RSC ADVANCES
卷 3, 期 42, 页码 19639-19656

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ROYAL SOC CHEMISTRY
DOI: 10.1039/c3ra42566e

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资金

  1. National Natural Science Foundation of China [21107106]
  2. Strategic Priority Research Program of the Chinese Academy of Sciences [XDB05050500]
  3. National Key Technology R&D Program of the Ministry of Science and Technology [2011BAZ01960]
  4. National Basic Research Program of China [2010CB732300]
  5. program of Innovation Team of the Bureau of Ningbo Science and Technology [201182001]

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SBA-16 silica with intact surface hydroxyl groups was quickly obtained (5 min) via a fast-microwave-assisted method, and further adopted as an efficient template for the synthesis of three-dimensional (3D) ordered mesoporous CuOx-CeO2 catalysts (htpCCx) through a simple and reproducible host-guest interaction. XRD, XPS, H-2-TPR, and Raman results reveal that many of the Cu2+ ions in htpCCx are incorporated into the CeO2 lattice, leading to the formation of a CuxCe1-xO2-delta solid solution, which produces a large number of oxygen vacancies and enhances the reducibility of the metal. The interaction of Cu and Ce is essential to the reaction as it maintains the Cu2+/Cu1+ and Ce4+/Ce3+ redox couples. The catalyst has a 3D mesostructure and possesses remarkably enhanced low-temperature activity for the combustion of epichlorohydrin. HtpCC20 has been identified as the most powerful catalyst for this reaction, with the reaction rate at 165 degrees C being about 6.3 and 33.3 times higher than those of catalysts synthesized using conventional incipient impregnation and thermal combustion methods, respectively. Furthermore, htpCC20 shows superior CO2 selectivity (>99%) and stability (no deactivation occurs after 50 h reaction). It is believed that the dispersion of the active phase, density of surface active oxygen, and low-temperature reducibility are the dominant factors governing the catalytic performance.

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