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Realization of high photocatalytic hydrogen generation activity by nanostructured Ga1-xZnxO1-zNz solid-solution without co-catalyst

机译:纳米结构的Ga1-xZnxO1-zNz固溶体在没有助催化剂的情况下实现高光催化制氢活性

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摘要

Photocatalysis requires light absorption as well as efficient extraction of the photo-generated electron hole pairs to chemically active sites. To avoid electron hole recombination, we need tailored nanostructures which can demonstrate novel light absorption and thermodynamic properties. This work shows that band gap modificationarrowing due to the formation of solid solution along with an increased surface area of the nanostructures are ideal for solar harvesting and is a self sufficient photocatalytic agent even in absence of a co-catalyst. The present study suggests that the rate of H-2 production for GaN was negligible and it increased to 32.43 mu mol/g/h for the solid solution under visible light irradiation (>400 nm) even in the absence of a co-catalyst. The apparent quantum yield (AQY) efficiency of H-2 evolution was found to be 0.8%. This highly desirable increased H-2 generation activity is attributed to the additional linewidth broadening in the photoluminescence spectra of nanostructured wurtzite Ga1-xZnxO1-zNz solid-solution due to Ga/Zn and N/O interdiffusion giving rise to a modified bandgap and N2p-O2p interaction in the lattice. These inferences are also corroborated by diffuse reflectance spectra of the samples. For the first time, origin of hitherto unreported weak features appearing in the low energy Raman spectrum is also discussed. A series of characterization tools including structural, microstructural, optical, spectroscopic and Photocatalytic hydrogen production studies were employed to support our claim. Copyright (C) 2015, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
机译:光催化需要光吸收以及将光生电子空穴对有效提取到化学活性位点。为了避免电子空穴复合,我们需要量身定制的纳米结构,这些结构可以显示出新颖的光吸收和热力学性质。这项工作表明,由于固溶体的形成以及纳米结构表面积的增加,带隙的改变/变窄是太阳能收集的理想选择,即使在没有助催化剂的情况下,也是自足的光催化剂。本研究表明,GaN的H-2生成速率可忽略不计,即使在没有助催化剂的情况下,在可见光照射(> 400 nm)下固溶体的H-2生成速率也提高到32.43μmol/ g / h。发现H-2演化的表观量子产率(AQY)效率为0.8%。这种高度期望的H-2生成活性增加归因于Ga / Zn和N / O互扩散导致纳米结构纤锌矿Ga1-xZnxO1-zNz固溶体的光致发光光谱中的额外线宽加宽,从而产生了改进的带隙和N2p-晶格中的O2p相互作用。样本的漫反射光谱也证实了这些推论。首次还讨论了迄今为止在低能拉曼光谱中未报道的弱特征的起源。我们采用了一系列表征工具,包括结构,微结构,光学,光谱和光催化制氢研究来支持我们的主张。 Hydrogen Energy Publications,LLC版权所有(C)2015。由Elsevier Ltd.出版。保留所有权利。

著录项

  • 来源
    《International journal of hydrogen energy》 |2015年第40期|13901-13908|共8页
  • 作者单位

    Anna Univ, Ctr Crystal Growth, Madras 600025, Tamil Nadu, India;

    Anna Univ, Ctr Crystal Growth, Madras 600025, Tamil Nadu, India;

    Anna Univ, Ctr Crystal Growth, Madras 600025, Tamil Nadu, India;

    Indira Gandhi Ctr Atom Res, Mat Sci Grp, Kalpakkam 603102, Tamil Nadu, India;

    Indira Gandhi Ctr Atom Res, Mat Sci Grp, Kalpakkam 603102, Tamil Nadu, India;

    Indira Gandhi Ctr Atom Res, Mat Sci Grp, Surface & Nanosci Div, Kalpakkam 603102, Tamil Nadu, India;

    Anna Univ, Ctr Crystal Growth, Madras 600025, Tamil Nadu, India;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    Nanostructures; Photocatalysis; Anomalous Raman modes; Band gap;

    机译:纳米结构;光催化;拉曼模态;带隙;

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