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用于可见光下高效降解苯的TiO光催化剂的N-H和H-N共掺杂机理研究

Mechanistic study of N-H- and H-N-codoping of a TiO photocatalyst for efficient degradation of benzene under visible light.

作者信息

Li Minghui, Song Wulin, Zeng Lei, Zeng Dawen, Xie Changsheng, Yang Qun

机构信息

State Key Laboratory of Materials Processing and Die & Mould Technology, Huazhong University of Science and Technology Wuhan 430074 P. R. China

Analytical and Testing Center, Huazhong University of Science and Technology P. R. China.

出版信息

RSC Adv. 2020 Jan 15;10(5):2757-2766. doi: 10.1039/c9ra09661b. eCollection 2020 Jan 14.

Abstract

Non-metal codoping including nitrogen (N) and hydrogen (H) codoping has been emerging as an effective way to improve the performance of anatase TiO in solar cell, fuel conversion and pollutant degradation. However, the mechanism of the synergistic effect of N doping and H doping on TiO is still far from thorough. In this paper, N and H codoped TiO nanoparticles are obtained by N doping in ammonia and then H doping in hydrogen gas, which achieves substantially boosted efficiency and reaction rate in the photocatalytic degradation of benzene under visible light excitation. The superiority of the N-H-TiO photocatalyst was fully elaborated by comparing with H-N-TiO, which was obtained by thermal treating in H and then NH. The reaction rate of N-H-TiO in the photocatalytic degradation of benzene was nearly 2 times that of H-N-TiO, ∼7 times higher than that of pristine TiO. Furthermore, the cycling test revealed the high repeatability and stability of the N-H-TiO photocatalyst. The excellent performance N-H-TiO was attributed to an adequate concentration of NH defects occupying interstitial sites of the TiO structure and a disordered surface layer introduced by annealing in NH and H successively. The synergistic effect of N-H-codoping also increased the separation and migration of electron-hole pairs triggering a photoinduced redox reaction on the surface of TiO.

摘要

包括氮(N)和氢(H)共掺杂在内的非金属共掺杂已成为提高锐钛矿型TiO在太阳能电池、燃料转化和污染物降解方面性能的有效方法。然而,N掺杂和H掺杂对TiO协同作用的机制仍远未彻底明晰。本文通过在氨气中进行N掺杂,然后在氢气中进行H掺杂,制备出N和H共掺杂的TiO纳米颗粒,其在可见光激发下对苯的光催化降解中实现了效率和反应速率的显著提高。通过与先在氢气中然后在氨气中热处理得到的H-N-TiO对比,充分阐述了N-H-TiO光催化剂的优越性。N-H-TiO在苯的光催化降解中的反应速率几乎是H-N-TiO的2倍,比原始TiO高约7倍。此外,循环测试表明N-H-TiO光催化剂具有高重复性和稳定性。N-H-TiO的优异性能归因于适量浓度的NH缺陷占据了TiO结构的间隙位置以及先后在氨气和氢气中退火引入的无序表面层。N-H共掺杂的协同效应还增加了电子-空穴对的分离和迁移,从而引发了TiO表面的光致氧化还原反应。

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