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Exploring the mechanism of a pure and amorphous black-blue TiO2:H thin film as a photoanode in water splitting
Nano Energy ( IF 16.8 ) Pub Date : 2017-10-28 , DOI: 10.1016/j.nanoen.2017.10.062
Junhui Liang , Ning Wang , Qixing Zhang , Bofei Liu , Xiangbin Kong , Changchun Wei , Dekun Zhang , Baojie Yan , Ying Zhao , Xiaodan Zhang

The use of amorphous disordered surface layers on TiO2 nanocrystals prepared by hydrogenated post-treatment has been proven to be an effective approach for enhancing the light absorption and photocatalytic activity of TiO2 photoanodes. However, the mechanism underlying the enhanced optical-electrical performance caused by the hydrogenated amorphous shell has still not been fully unveiled. Herein, to explore the mechanism without the effect of the crystalline structure, a pure, amorphous hydrogen-doped TiO2 (a-TiO2:H) film was prepared using a magnetron sputtering technique under reactive hydrogen plasma. We propose that the cooperative effects of the extended mid-gap states and valence band tail are responsible for the enhanced visible and near-infrared optical absorption. In addition, the doped H acts as a shallow donor to provide carriers and shift the Fermi level to the conduction band, ultimately accelerating charge transport and transfer at the semiconductor/electrolyte interface. Finally, the photoconversion efficiency of a-TiO2:H was improved one order of magnitude compared to undoped a-TiO2:H. Through the investigation of a-TiO2:H, we gained further insight into black TiO2. In addition, we believe our a-TiO2:H film grown at room temperature opens new opportunities for a broad range of applications, including PEC water splitting, supercapacitors, dye-sensitized solar cells, and perovskite solar cells.



中文翻译:

探索纯无定形黑蓝色TiO 2:H薄膜在水分解中作为光阳极的机理

已经证明在通过氢化后处理制备的TiO 2纳米晶体上使用无定形无序表面层是增强TiO 2光阳极的光吸收和光催化活性的有效方法。但是,由氢化非晶壳引起的增强光电性能的机理仍未完全揭示。在此,为探索不受晶体结构影响的机理,纯净,无定形的氢掺杂TiO 2(a-TiO 2:H)膜是在反应性氢等离子体下使用磁控溅射技术制备的。我们建议,扩展的中间能隙状态和价带尾的协同效应是导致可见光和近红外光吸收增强的原因。此外,掺杂的H充当浅施主,以提供载流子并将费米能级移至导带,最终加速了半导体/电解质界面上的电荷传输和转移。最后,-TiO 2的光转换效率2:H得到改善一个数量级相比无掺杂一个-TIO 2:H。通过对a-TiO 2:H的研究,我们对黑色TiO 2有了进一步的了解。此外,我们相信我们的a-TiO 2在室温下生长的:H膜为广泛的应用提供了新的机会,包括PEC水分解,超级电容器,染料敏化太阳能电池和钙钛矿太阳能电池。

更新日期:2017-10-28
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