SBA-15负载磷钼钒酸构筑高效室温光热氧化脱硫催化剂  

SBA-15-Supported Molybdovanadophosphoric Acid Photothermal Catalysts for Efficient Oxidation Desulfurization at Room Temperature

作　　者：祝梦春 李齐齐 田洪瑞 毕研峰 ZHU Meng-Chun;LI Qi-Qi;TIAN Hong-Rui;BI Yan-Feng(School of Petrochemical Engineering,Liaoning Petrochemical University,Fushun 113001,China)

机构地区：[1]辽宁石油化工大学石油化工学院,抚顺113001

出　　处：《应用化学》2024年第10期1469-1480,共12页Chinese Journal of Applied Chemistry

基　　金：国家自然科学基金(No.91961110)资助。

摘　　要：采用等体积浸渍法在介孔SBA-15负载SBA-15的质量分数X%(X=10,20,30,40,50)Keggin型杂多酸H_(4)PMo_(11)VO_(40)(PMoV),制备系列催化剂X%PMoV,用于室温条件下可见光光热氧化脱硫。通过比表面积分析(BET)、傅里叶变换红外光谱仪(FT-IR)、X射线衍射仪(XRD)、透射电子显微镜(TEM)、X射线电子能谱分析仪(XPS)和紫外可见分光光度计(UV-Vis)对催化剂进行了表征。催化剂在乙腈溶剂中的表现出了光热转换能力,且光热转化效果随活性组分负载量增加而变强。以H2O2为氧化剂,二苯并噻吩(DBT)为例的模型油中,对催化剂光热氧化脱除硫进行了研究。研究表明,催化剂对DBT具有光催化和光驱动热催化的协同氧化脱硫能力。得益于活性组分PMoV在载体SBA-15孔道内的有效负载,当负载量为30%时,催化剂具有较好的循环稳定性和底物氧化产物选择性。催化剂的光热催化脱硫策略也适用于其它噻吩类衍生物以及硫醚类化合物。此研究为利用可见光吸收活性组分负载于分子筛,用于光驱动光催化和热催化脱硫应用提供了一种新的思路。A series of catalysts,X%PMoV(X=10,20,30,40,50),were prepared through loading X%(mass fraction of SBA-15)Keggin-type H_(4)PMo_(11)VO_(40)(PMoV)on mesoporous SBA-15 by incipient-wetness impregnation method,which were utilized as visible-light catalysts for photothermal oxidation desulfurization at room temperature.The catalysts were characterized by brunauer Emmett Trller(BET),fourier transform infrared spectroscopy(FT-IR),powder X-ray diffration(PXRD),transmission electron microscope(TEM),X-ray photoelectron spectroscopy(XPS),and UV-Vis.X%PMoV catalysts showed photothermal conversion ability in acetonitrile solvent,and the photothermal conversion efficiency increased with the increase of PMoV.The oxidation desulfurization experiment of dibenzothiophene(DBT,as an example)was carried out in model oil with oxidant H2O2.The results show that the catalyst has the synergistic oxidative desulfurization ability of photocatalysis and photo-driven thermal catalysis on DBT.Due to the effective load of the active PMoV in the SBA-15 channels,the catalyst has good cyclic stability and substrate oxidation product selectivity when the load is 30%.The photothermal catalytic desulfurization strategy is also applicable for other thiophene derivatives and thioether compounds.This paper provides a new idea for using visible-light absorption active components loaded on zeolite for photocatalytic and thermocatalytic desulfurization applications.

关 键 词：磷钼钒酸 SBA-15 光热转换 氧化脱硫 

分 类 号：O643.3[理学—物理化学]