Effect of carbon-interaction on structure-photoactivity of Cu doped amorphous TiO2 catalysts for visible-light-oriented oxidative desulphurization of dibenzothiophene
Effect of carbon-interaction on structure-photoactivity of Cu doped amorphous TiO2 catalysts for visible-light-oriented oxidative desulphurization of dibenzothiophene
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DOI：
10.1016/j.fuel.2017.12.035
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发表时间：
2018-03
期刊：
影响因子：
7.4
通讯作者：
C. Hitam;A. A. Jalil-A.;S. Triwahyono;A.F.A. Rahman;N. Hassan;N. F. Khusnun;S. F. Jamian;C. R. Mamat;W. Nabgan;W. Nabgan;A. Ahmad
中科院分区：
文献类型：
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作者：
C. Hitam;A. A. Jalil-A.;S. Triwahyono;A.F.A. Rahman;N. Hassan;N. F. Khusnun;S. F. Jamian;C. R. Mamat;W. Nabgan;W. Nabgan;A. Ahmad
采用溶胶-凝胶法制备了非晶态TiO 2（AT），并通过电化学方法引入Cu，制备了CuO/TiO 2（CAT）催化剂。采用XRD、N2物理吸附、FTIR、TEM、EDX、XPS、ESR和UV-Vis DRS等手段对催化剂进行了表征，结果表明，不同钛前驱体的使用对催化剂的物化性能有较大影响。在添加铜的过程中，钛前驱体一锅自掺杂碳，可显著提高CAT对二苯并噻吩（DBT）氧化脱硫的光催化活性。15 CATTBOTi的最佳性能主要归因于最小的带隙和较高的O-Ti-C和Ti-O-C键数以及适量的Ti 3+表面缺陷（TSD）。这些上述性质提供了良好的电子-空穴对的迁移率和/或捕获电子以增强在可见光照射下的光活性。动力学研究表明，DBT光催化氧化脱硫反应符合准一级动力学Langmuir-Hinshelwood模型，其中吸附是控制步骤。据信，这些结果可以有助于合成用于许多应用的各种负载型催化剂，特别是用于去除燃料油中的含硫化合物。
Amorphous TiO2(AT) was successfully prepared via the sol-gel technique, using different titanium sources followed by incorporation of copper via the electrochemical method to give CuO/TiO2(CAT) catalysts. The catalysts were characterized via XRD, N2physisorption, FTIR, TEM, EDX, XPS, ESR and UV–Vis DRS. The results verified that the use of different titanium precursors have profound effect on the physicochemical properties of the AT catalysts. Further one-pot self-doping carbon from titanium precursor during the addition of copper could greatly enhanced the photocatalytic activity of CAT on the oxidative desulphurization of dibenzothiophene (DBT). 15 CATTBOTexhibited the best performance mainly due to the narrowest band gap and higher numbers of O–Ti–C and Ti–O–C bonds, as well as appropriate amount of Ti3+surface defects (TSD). These abovementioned properties offered good mobility of electron-hole pairs and/or trap the electrons for enhancement of photoactivity under irradiation of visible light. Kinetic studies showed that the photocatalytic oxidative desulphurization of DBT followed the pseudo-first order Langmuir-Hinshelwood model, where the adsorption was the controlling step. It is believed that these results could contribute to the synthesis of various supported catalysts for numerous applications specifically in removal of sulphur containing compounds in fuel oils.