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通过反向级联载流子转移实现高效光催化析氢

Effective Photocatalytic Hydrogen Evolution by Cascadal Carrier Transfer in the Reverse Direction.

作者信息

Nagakawa Haruki, Ochiai Tsuyoshi, Takekuma Yuya, Konuma Seiji, Nagata Morio

机构信息

Department of Industrial Chemistry, Graduate School of Engineering, Tokyo University of Science, 12-1 Ichigayafunagawara-cho, Shinjuku-ku, Tokyo 162-0826, Japan.

Photocatalyst Group, Research and Development Department, Local Independent Administrative Agency Kanagawa Institute of Industrial Science and TEChnology (KISTEC), Kanagawa 213-0012, Japan.

出版信息

ACS Omega. 2018 Oct 8;3(10):12770-12777. doi: 10.1021/acsomega.8b02449. eCollection 2018 Oct 31.

Abstract

Visible-light-responsive photocatalysts used in the highly efficient hydrogen production exhibit several disadvantages such as photocorrosion and fast recombination. Because of the potential important applications of such catalysts, it is crucial that a simple, effective solution is developed. In this respect, in this study, we combined SiC (β modification) and TiO with CdS to overcome the challenges of photocorrosion and fast recombination of CdS. Notably, we found that when irradiated with visible light, CdS was excited, and the excited electrons moved to the conduction band of TiO, thereby increasing the efficiency of charge separation. In addition, by moving the holes generated on CdS to the valence band of SiC, in the opposite direction of TiO, photocorrosion and fast recombination were prevented. As a result, in the sulfide solution, the CdS/SiC composite catalyst exhibited 4.3 times higher hydrogen generation ability than pure CdS. Moreover, this effect was enhanced with the addition of TiO, giving 10.8 times higher hydrogen generation ability for the CdS/SiC/TiO catalyst. Notably, the most efficient catalyst, which was obtained by depositing Pt as a cocatalyst, exhibited 1.09 mmol g h hydrogen generation ability and an apparent quantum yield of 24.8%. Because water reduction proceeded on the TiO surface and oxidative sulfide decomposition proceeded on the SiC surface, the exposure of CdS to the solution was unnecessary, and X-ray photoelectron spectroscopy confirmed that photocorrosion was successfully suppressed. Thus, we believe that the effective composite photocatalyst construction method presented herein can also be applied to other visible-light-responsive powder photocatalysts having the same disadvantages as CdS, thereby improving the efficiency of such catalysts.

摘要

用于高效制氢的可见光响应型光催化剂存在光腐蚀和快速复合等几个缺点。由于此类催化剂具有潜在的重要应用,开发一种简单有效的解决方案至关重要。在这方面,在本研究中,我们将SiC(β型)和TiO与CdS相结合,以克服CdS的光腐蚀和快速复合问题。值得注意的是,我们发现当用可见光照射时,CdS被激发,激发电子转移到TiO的导带,从而提高了电荷分离效率。此外,通过将CdS上产生的空穴沿与TiO相反的方向转移到SiC的价带,防止了光腐蚀和快速复合。结果,在硫化物溶液中,CdS/SiC复合催化剂的产氢能力比纯CdS高4.3倍。此外,添加TiO后这种效果得到增强,CdS/SiC/TiO催化剂的产氢能力提高到10.8倍。值得注意的是,通过沉积Pt作为助催化剂获得的最有效催化剂,其产氢能力为1.09 mmol g h,表观量子产率为24.8%。由于水还原在TiO表面进行,氧化硫化物分解在SiC表面进行,无需将CdS暴露于溶液中,X射线光电子能谱证实光腐蚀得到成功抑制。因此,我们认为本文提出的有效复合光催化剂构建方法也可应用于其他与CdS具有相同缺点的可见光响应型粉末光催化剂,从而提高此类催化剂的效率。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b30d/6645024/0d1f8fa1c27f/ao-2018-02449m_0001.jpg

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