4.6 Article

Tuning the Surface Structure of Nitrogen-Doped TiO2 Nanofibres-An Effective Method to Enhance Photocatalytic Activities of Visible-Light-Driven Green Synthesis and Degradation

期刊

CHEMISTRY-A EUROPEAN JOURNAL
卷 19, 期 18, 页码 5731-5741

出版社

WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201203961

关键词

doping; hydroamination; photochemistry; photocatalysts; SPR; visible light

资金

  1. Australian Research Council (ARC)

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Nitrogen-doped TiO2 nanofibres of anatase and TiO2(B) phases were synthesised by a reaction between titanate nanofibres of a layered structure and gaseous NH3 at 400700 degrees C, following a different mechanism than that for the direct nitrogen doping from TiO2. The surface of the N-doped TiO2 nanofibres can be tuned by facial calcination in air to remove the surface-bonded N species, whereas the core remains N doped. N-Doped TiO2 nanofibres, only after calcination in air, became effective photocatalysts for the decomposition of sulforhodamineB under visible-light irradiation. The surface-oxidised surface layer was proven to be very effective for organic molecule adsorption, and the activation of oxygen molecules, whereas the remaining N-doped interior of the fibres strongly absorbed visible light, resulting in the generation of electrons and holes. The N-doped nanofibres were also used as supports of gold nanoparticle (Au NP) photocatalysts for visible-light-driven hydroamination of phenylacetylene with aniline. Phenylacetylene was activated on the N-doped surface of the nanofibres and aniline on the Au NPs. The Au NPs adsorbed on N-doped TiO2(B) nanofibres exhibited much better conversion (80% of phenylacetylene) than when adsorbed on undoped fibres (46%) at 40 degrees C and 95% of the product is the desired imine. The surface N species can prevent the adsorption of O2 that is unfavourable for the hydroamination reaction, and thus, improve the photocatalytic activity. Removal of the surface N species resulted in a sharp decrease of the photocatalytic activity. These photocatalysts are feasible for practical applications, because they can be easily dispersed into solution and separated from a liquid by filtration, sedimentation or centrifugation due to their fibril morphology.

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