Miyauchi Masahiro, Irie Hiroshi, Liu Min, Qiu Xiaoqing, Yu Huogen, Sunada Kayano, Hashimoto Kazuhito
Graduate School of Science and Engineering, Tokyo Institute of Technology , 2-12-1 Ookayama, Meguro-ku, Tokyo 152-8552, Japan.
Clean Energy Research Center, University of Yamanashi , 4-3-11 Takeda, Kofu, Yamanashi 400-8511, Japan.
J Phys Chem Lett. 2016 Jan 7;7(1):75-84. doi: 10.1021/acs.jpclett.5b02041. Epub 2015 Dec 16.
Photocatalytic degradation of organic compounds requires photoexcited holes with strong oxidative power in the valence band (VB) of semiconductors. Although numerous types of doped semiconductors, such as nitrogen-doped TiO2, have been studied as visible-light-sensitive photocatalysts, the quantum yields of these materials were very low because of the limited oxidation power of holes in the nitrogen level above the VB. Recently, we developed visible-light-sensitive Cu(II) and Fe(III) nanocluster-grafted TiO2 using a facile impregnation method and demonstrated that visible-light absorption occurs at the interface between the nanoclusters and TiO2, as electrons in the VB of TiO2 are excited to the nanoclusters under visible-light irradiation. In addition, photogenerated holes in the VB of TiO2 efficiently oxidize organic contaminants, and the excited electrons that accumulate in nanoclusters facilitate the multielectron reduction of oxygen. Notably, Cu(II) and Fe(III) nanocluster-grafted TiO2 photocatalyst has the highest quantum yield among reported photocatalysts and has antiviral, self-cleaning, and air purification properties under illumination by indoor light fixtures equipped with white fluorescent bulbs or white light-emitting diodes.
有机化合物的光催化降解需要半导体价带(VB)中具有强氧化能力的光激发空穴。尽管已经研究了多种类型的掺杂半导体,如氮掺杂的TiO₂,作为可见光敏感的光催化剂,但由于价带上方氮能级中空穴的氧化能力有限,这些材料的量子产率非常低。最近,我们采用简便的浸渍法开发了可见光敏感的Cu(II)和Fe(III)纳米团簇接枝的TiO₂,并证明在可见光照射下,由于TiO₂价带中的电子被激发到纳米团簇上,在纳米团簇与TiO₂的界面处发生可见光吸收。此外,TiO₂价带中的光生空穴有效地氧化有机污染物,而积累在纳米团簇中的激发电子促进了氧的多电子还原。值得注意的是,Cu(II)和Fe(III)纳米团簇接枝的TiO₂光催化剂在已报道的光催化剂中具有最高的量子产率,并且在配备白色荧光灯泡或白色发光二极管的室内灯具照明下具有抗病毒、自清洁和空气净化性能。