阴离子无序及其对氧氮化物光活性半导体表面电子结构的影响

Anna Hartl, Ján Minár, Procopios Constantinou, Vladimir Roddatis, Fatima Alarab, Arnold M. Müller, Christof Vockenhuber, Thorsten Schmitt, Daniele Pergolesi, Thomas Lippert Vladimir N. Strocov, Nick A. Shepelin
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引用次数: 0

摘要

将太阳能转化为化学能并以氢的形式储存起来,作为一种可持续燃料为新兴技术提供动力,具有巨大的潜力。光活性氧化物是一种很有前途的材料,可将水分离成分子氧和氢。虽然最近的研究显示了氮的损失,但其与降低效率的关系还没有通过实验得到直接和系统的解决。在本研究中,我们证明了 BaTaO$_x$N$_y$ 的阴离子几何形状对其电子结构和功能特性的影响。通过实验离子散射、电子显微镜和光电子能谱研究,我们确定了 BaTaO$_x$N$_y$ 薄膜从块体到表面的阴离子组成。这进一步为模拟阴离子位点亚机构无序的带状结构计算提供了输入。结合我们的实验和计算方法,我们揭示了氮氧化物薄膜中与深度相关的元素组成,这导致了向下的带弯曲和半导特性向表面的丧失。在理想化系统之外,我们还证明了实际氮氧化物光阳极的电子特性与其性能之间的关系,为设计高效光电极和光催化剂以实现清洁制氢提供了指导。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Anionic disorder and its impact on the surface electronic structure of oxynitride photoactive semiconductors
The conversion of solar energy into chemical energy, stored in the form of hydrogen, bears enormous potential as a sustainable fuel for powering emerging technologies. Photoactive oxynitrides are promising materials for splitting water into molecular oxygen and hydrogen. However, one of the issues limiting widespread commercial use of oxynitrides is the degradation during operation. While recent studies have shown the loss of nitrogen, its relation to the reduced efficiency has not been directly and systematically addressed with experiments. In this study, we demonstrate the impact of the anionic stoichiometry of BaTaO$_x$N$_y$ on its electronic structure and functional properties. Through experimental ion scattering, electron microscopy, and photoelectron spectroscopy investigations, we determine the anionic composition ranging from the bulk towards the surface of BaTaO$_x$N$_y$ thin films. This further serves as input for band structure computations modeling the substitutional disorder of the anion sites. Combining our experimental and computational approaches, we reveal the depth-dependent elemental composition of oxynitride films, resulting in downward band bending and the loss of semiconducting character towards the surface. Extending beyond idealized systems, we demonstrate the relation between the electronic properties of real oxynitride photoanodes and their performance, providing guidelines for engineering highly efficient photoelectrodes and photocatalysts for clean hydrogen production.
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