狄璐,赵胜男,李新刚.表面活性剂修饰ZnIn2S4光催化甲苯选择性氧化[J].分子催化,2022,36(5):413-424
表面活性剂修饰ZnIn2S4光催化甲苯选择性氧化
Photocatalytic Selective Oxidation of Toluene over Surfactant-Modified ZnIn2S4
投稿时间:2022-06-23  修订日期:2022-08-03
DOI:10.16084/j.issn1001-3555.2022.05.001
中文关键词:  光催化  ZnIn2S4  硫缺陷  表面活性剂  甲苯氧化
英文关键词:photocatalysis  ZnIn2S4  sulfur vacancies  surfactant  toluene oxidation
基金项目:国家自然科学基金项目(21905144);南开大学2022年自制实验教学仪器设备类项目(气态流动鼓泡反应器的研制)
作者单位E-mail
狄璐 南开大学 材料科学与工程学院, 天津 300350 dilu@nankai.edu.cn 
赵胜男 天津大学 化工学院, 天津 300354
山东寿光巨能金玉米开发有限公司, 山东 寿光 262700 
zhaoshengnan@tju.edu.cn 
李新刚 天津大学 化工学院, 天津 300354  
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中文摘要:
      采用溶剂热合成法,借助十六烷基三甲基溴化铵(CTAB)和十八烷基三甲基溴化铵(STAB)的修饰合成了富含硫缺陷的ZnIn2S4-CTAB和ZnIn2S4-STAB光催化剂.通过透射电镜、X射线衍射、紫外可见漫反射光谱、电子顺磁共振和光电化学性能测试对所有样品进行了表征,并通过光催化甲苯氧化反应测试样品的催化活性.活性结果表明ZnIn2S4-CTAB和ZnIn2S4-STAB上甲苯转化速率分别达到795和1053 μmol·gcat-1·h-1,是未修饰ZnIn2S4-Blank催化剂的4倍和5倍,同时目标产物苯甲醛选择性均大于92%.机理研究发现,表面活性剂修饰后的ZnIn2S4-CTAB和ZnIn2S4-STAB较ZnIn2S4-Blank具有更高浓度的硫缺陷.硫缺陷通过捕获电子促进了光生载流子的分离与利用,显著提高了ZnIn2S4-CTAB和ZnIn2S4-STAB的光催化甲苯选择性氧化制苯甲醛的活性.
英文摘要:
      ZnIn2S4-CTAB and ZnIn2S4-STAB photocatalysts with rich sulfur vacancies were prepared by a hydrothermal method via the modification of ZnIn2S4 with cetyltrimethylammonium bromide (CTAB) and stearyl trimethylammonium bromide (STAB). All samples were characterized by transmission electron microscopy, X-ray diffraction, UV-vis diffuse reflectance absorption spectroscopy, electron paramagnetic resonance and photoelectrochemical performance test. The photocatalytic selective oxidation of toluene was conducted over all ZnIn2S4 samples. The conversion rates of toluene over ZnIn2S4-CTAB and ZnIn2S4-STAB reached 795 and 1053 μmol·gcat-1 ·h-1, respectively, which were 4 and 5 times higher than ZnIn2S4-Blank. More importantly, the selectivity of benzaldehyde was above 92% over both ZnIn2S4-CTAB and ZnIn2S4-STAB. The mechanism studies demonstrated that surfactant-modified ZnIn2S4-CTAB and ZnIn2S4-STAB displayed higher contents of sulfur vacancies than the unmodified ZnIn2S4-Blank. The capture of photogenerated electrons by sulfur vacancies promoted the separation efficiency of photogenerated carriers, thereby achieving efficient photocatalytic selective oxidation of toluene.
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