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首页> 外文期刊>Advanced Functional Materials >Evidence and Effect of Photogenerated Charge Transfer for Enhanced Photocatalysis in WO3/TiO2 Heterojunction Films: A Computational and Experimental Study
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Evidence and Effect of Photogenerated Charge Transfer for Enhanced Photocatalysis in WO3/TiO2 Heterojunction Films: A Computational and Experimental Study

机译：WO3 / TiO2异质结薄膜中光生电荷转移增强光催化的证据和作用：计算和实验研究

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摘要

Semiconductor heterojunctions are used in a wide range of applications including catalysis, sensors, and solar-to-chemical energy conversion devices. These materials can spatially separate photogenerated charge across the heterojunction boundary, inhibiting recombination processes and synergistically enhancing their performance beyond the individual components. In this work, the WO3/TiO2 heterojunction grown by chemical vapor deposition is investigated. This consists of a highly nanostructured WO3 layer of vertically aligned nanorods that is then coated with a conformal layer of TiO2. This heterojunction shows an unusual electron transfer process, where photogenerated electrons move from the WO3 layer into TiO2. State-of-the-art hybrid density functional theory and hard X-ray photoelectron spectroscopy are used to elucidate the electronic interaction at the WO3/TiO2 interface. Transient absorption spectroscopy shows that recombination is substantially reduced, extending both the lifetime and population of photogenerated charges into timescales relevant to most photocatalytic processes. This increases the photocatalytic efficiency of the material, which is among the highest ever reported for a thin film. In allying computational and experimental methods, this is believed to be an ideal strategy for determining the band alignment in metal oxide heterojunction systems.
机译：半导体异质结的应用范围很广，包括催化，传感器和日光化学能转换装置。这些材料可以在空间上跨异质结边界分离光生电荷，从而抑制重组过程，并协同增强其性能，超越了单个组分。在这项工作中，研究了通过化学气相沉积生长的WO3 / TiO2异质结。它由垂直排列的纳米棒的高度纳米结构的WO3层组成，然后涂覆有TiO2的保形层。这种异质结显示出不寻常的电子传输过程，其中光生电子从WO3层移动到TiO2中。最新的混合密度泛函理论和硬X射线光电子能谱被用来阐明WO3 / TiO2界面的电子相互作用。瞬态吸收光谱显示重组显着减少，将光生电荷的寿命和种群延长到与大多数光催化过程相关的时标。这提高了材料的光催化效率，这是有史以来薄膜最高的。在各种计算和实验方法中，这被认为是确定金属氧化物异质结系统中能带排列的理想策略。

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  • 来源
    《Advanced Functional Materials》 |2017年第18期|1605413.1-1605413.10|共10页
  • 作者

    Sotelo-Vazquez Carlos; Quesada-Cabrera Raul; Ling Min; Scanlon David O.; Kafizas Andreas; Thakur Pardeep Kumar; Lee Tien-Lin; Taylor Alaric; Watson Graeme W.; Palgrave Robert G.; Durrant James R.; Blackman Christopher S.; Parkin Ivan P.;

  • 作者单位

    UCL, Dept Chem, 20 Gordon St, London WC1H 0AJ, England;

    UCL, Dept Chem, 20 Gordon St, London WC1H 0AJ, England;

    UCL, Dept Chem, 20 Gordon St, London WC1H 0AJ, England;

    UCL, Dept Chem, 20 Gordon St, London WC1H 0AJ, England|Diamond Light Source Ltd, Harwell Sci & Innovat Campus, Didcot OX11 0DE, Oxon, England;

    UCL, Dept Chem, 20 Gordon St, London WC1H 0AJ, England|Imperial Coll London, Dept Chem, Exhibit Rd, London SW7 2AZ, England;

    Diamond Light Source Ltd, Harwell Sci & Innovat Campus, Didcot OX11 0DE, Oxon, England;

    Diamond Light Source Ltd, Harwell Sci & Innovat Campus, Didcot OX11 0DE, Oxon, England;

    UCL, Dept Elect & Elect Engn, Torrington Pl, London WC1E 7JE, England;

    Trinity Coll Dublin, Sch Chem, Dublin 2, Ireland|Trinity Coll Dublin, CRANN Inst, Dublin 2, Ireland;

    UCL, Dept Chem, 20 Gordon St, London WC1H 0AJ, England;

    Imperial Coll London, Dept Chem, Exhibit Rd, London SW7 2AZ, England;

    UCL, Dept Chem, 20 Gordon St, London WC1H 0AJ, England;

    UCL, Dept Chem, 20 Gordon St, London WC1H 0AJ, England;

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