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介孔ZnO/TiO-SiO复合材料的合成及其在无额外氧化剂添加的光催化吸附脱硫中的应用。

Synthesis of mesoporous ZnO/TiO-SiO composite material and its application in photocatalytic adsorption desulfurization without the addition of an extra oxidant.

作者信息

Zhou Kangdi, Ding Yongcong, Zhang Linfeng, Wu Huadong, Guo Jia

机构信息

Key Laboratory of Green Chemical Process of Ministry of Education, Hubei Key Laboratory of Novel Chemical Reactor and Green Chemical Technology, Wuhan Institute of Technology, Wuhan 430073, P. R. China.

出版信息

Dalton Trans. 2020 Feb 5;49(5):1600-1612. doi: 10.1039/c9dt04454j.

Abstract

Photocatalytic adsorption desulfurization (PADS) technology has attracted enormous attention in the deep desulfurization field. Therefore, a good material with high photocatalytic activity and adsorption capacity toward organic sulfide is desirable. Herein, mesoporous ZnO/TiO2-SiO2 (ZTS) was synthesized for the first time and successfully applied in the photocatalytic desulfurization of dibenzothiophene (DBT). The composite materials were characterized by means of X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), N2-physisorption, transmission electron microscopy (TEM), UV-Vis diffusive reflectance spectra (UV-Vis DRS), X-ray photo-electron spectroscopy (XPS), photoluminescence (PL) and electron spin resonance (ESR). The results show that the doping of TiO2 promotes the photocatalytic and adsorption abilities of the catalysts dramatically. ZTS-3 with Si/Ti = 3 exhibits the best photocatalytic desulfurization activity compared with other proportions of titanium doping. The final DBT conversion can reach 97%, and the maximum adsorption of DBT over ZTS-3 is 47 mg-S per g-cat. The photocatalytic test indicates that the remarkable photocatalytic activity of ZTS is due to the formation of a heterojunction by the interaction of ZnO and TiO2, which can successfully expand solar light absorption, improving the charge separation efficiency and inhibiting the recombination of photocatalytic electron-hole pairs. Moreover, no extra oxidants (such as O2, H2O2 or an organic oxidant) were added, which is highly beneficial for the consequent treatment of the fuel and can reduce the processing cost markedly.

摘要

光催化吸附脱硫(PADS)技术在深度脱硫领域引起了极大关注。因此,需要一种对有机硫化物具有高光催化活性和吸附能力的优良材料。在此,首次合成了介孔ZnO/TiO2-SiO2(ZTS)并成功应用于二苯并噻吩(DBT)的光催化脱硫。通过X射线衍射(XRD)、场发射扫描电子显微镜(FESEM)、N2物理吸附、透射电子显微镜(TEM)、紫外-可见漫反射光谱(UV-Vis DRS)、X射线光电子能谱(XPS)、光致发光(PL)和电子自旋共振(ESR)对复合材料进行了表征。结果表明,TiO2的掺杂显著提高了催化剂的光催化和吸附能力。与其他钛掺杂比例相比,Si/Ti = 3的ZTS-3表现出最佳的光催化脱硫活性。最终DBT转化率可达97%,ZTS-3对DBT的最大吸附量为每克催化剂47 mg-S。光催化测试表明,ZTS显著的光催化活性归因于ZnO和TiO2相互作用形成的异质结,其可以成功扩展太阳光吸收,提高电荷分离效率并抑制光催化电子-空穴对的复合。此外,未添加额外的氧化剂(如O2、H2O2或有机氧化剂),这对后续燃料处理非常有利,并且可以显著降低处理成本。

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