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Fabrication of titanosilicate pillared MFI zeolites with tailored catalytic activity
Frontiers of Chemical Science and Engineering ( IF 4.3 ) Pub Date : 2020-01-04 , DOI: 10.1007/s11705-019-1859-3
Baoyu Liu , Qiaowen Mu , Jiajin Huang , Wei Tan , Jing Xiao

Titanosilicate pillared MFI zeolite nanosheets were successfully synthesized by infiltrating the mixed tetraethyl orthosilicate (TEOS)/tetrabutyl orthotitanate (TBOT) solvent into the gallery space between adjacent MFI zeolite layers. The obtained zeolite catalysts were characterized using powder X-ray diffraction, N2 adsorption/desorption isotherms, scanning electron microscopy, transmission electron microscopy, ultraviolet-visible spectroscopy, X-ray photoelectron spectroscopy, and Fourier-transform infrared spectroscopy techniques. The H2O2 oxidation of dibenzothiophene (DBT) was used to evaluate the catalytic performance of the obtained titanosilicate pillared MFI zeolites. The conversion of DBT and selectivity of dibenzothiophene sulfone (DBTS) were most affected by the textural properties of the zeolites. This was attributed to the DBT and DBTS molecules being larger than micropores of the MFI zeolites. The conversion of DBT and yield of DBTS could be systematically tailored by tuning the molar ratio of the TEOS/TBOT solvent. These results implied that a balance between the meso- and microporosity of zeolites and tetrahedrally coordinated Ti (IV) active sites of titanosilicate pillars can be achieved for the preparation of desired catalysts during the oxidation of bulk S compounds.



中文翻译:

具有定制催化活性的钛硅酸盐柱状MFI沸石的制备

通过将混合的原硅酸四乙酯(TEOS)/原钛酸四丁酯(TBOT)溶剂渗透到相邻MFI沸石层之间的通道空间中,成功合成了钛硅酸盐柱状MFI沸石纳米片。使用粉末X射线衍射,N 2吸附/解吸等温线,扫描电子显微镜,透射电子显微镜,紫外可见光谱,X射线光电子光谱和傅里叶变换红外光谱技术对获得的沸石催化剂进行表征。H 2 O 2使用二苯并噻吩的氧化(DBT)评估所得的钛硅酸盐柱状MFI沸石的催化性能。DBT的转化率和二苯并噻吩砜(DBTS)的选择性受沸石的结构性质影响最大。这归因于DBT和DBTS分子大于MFI沸石的微孔。通过调节TEOS / TBOT溶剂的摩尔比,可以系统地调整DBT的转化率和DBTS的产率。这些结果表明,在介孔S化合物的氧化过程中,沸石的介孔和微孔率与钛硅酸盐柱的四面体配位的Ti(IV)活性位点之间可以达到平衡,以制备所需的催化剂。

更新日期:2020-01-04
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