CuWO4/SBA-15催化剂的制备及其光催化氧化脱硫性能  

Preparation of the CuWO4/SBA-15 catalyst and its performance in the photocatalytic oxidation desulfurization

作　　者：李剑[1] 王雪莹 黄鑫[2] 洪帅领 杨丽娜[1] LI Jian;WANG Xue-ying;HUANG Xin;HONG Shuai-ling;YANG Li-na(College of Chemistry,Chemical Engineering and Environmental Engineering,Liaoning Shihua University,Fushun 113001,China;Sinopec Yanshan Petrochemical Company,Beijing 102500,China)

机构地区：[1]辽宁石油化工大学化学化工与环境学部,辽宁抚顺113001 [2]中国石化燕山石化公司,北京102500

出　　处：《燃料化学学报》2020年第5期632-640,I0008,共10页Journal of Fuel Chemistry and Technology

基　　金：辽宁省高等学校杰出青年学者成长计划项目(LJQ2015062);辽宁省科学技术厅项目(20170540585);辽宁省教育厅项目(L2015296,L2016018)资助。

摘　　要：以CuWO4为活性组分、SBA-15介孔分子筛为载体,制备CuWO4/SBA-15催化剂,利用XRD、N2吸附-脱附、FT-IR、UV-vis、SEM、EDS和TEM对催化剂进行表征分析;以二苯并噻吩(DBT)的十二烷溶液为模拟油,研究了CuWO4/SBA-15的光催化氧化脱硫(PODS)性能。结果表明,CuWO4/SBA-15保持了载体高度有序的二维六方介孔结构,活性组分分布均匀,且随负载量增加,其比表面积、孔径和孔容依次减小。与CuWO4相比,CuWO4/SBA-15的UV-vis吸收边界蓝移,禁带宽度增加。以二苯并噻吩(DBT)的十二烷溶液为模拟油,评价催化剂的光催化氧化脱硫(PODS)性能。当CuWO4与SiO2质量比为0.07,催化剂用量为3%,O/S物质的量比为10∶1,剂油体积比为1∶1,光照反应100 min时,催化剂脱硫率最高,可达到81.5%,明显高于CuWO4,催化剂重复使用六次后,活性没有明显下降。在PODS反应过程中,·OH和h+是反应的主要活性物种。The CuWO4/SBA-15 catalyst was prepared with CuWO 4 as the active composite and mesoporous SBA-15 molecular sieve as the support and characterized by XRD,N 2 adsorption and desorption,FT-IR,UV-vis,SEM,EDS and TEM;the performance of CuWO4/SBA-15 catalyst in the photocatalytic oxidation desulfurization(PODS)was investigated by using the dodecane solution of dibenzothiophene(DBT)as the model fuel.The results show that the CuWO4/SBA-15 catalyst can maintain the two-dimensional hexagonal mesoporous structure of the support and the active component is evenly distributed on the support;the surface area,pore size and pore volume of the CuWO4/SBA-15 catalyst decrease with an increase in the amount of active component.Compared with CuWO4,the CuWO4/SBA-15 catalyst displays a blue shift in absorption boundary of UV-vis spectra and an increase of the band gap.With a CuWO4/SiO2 mass ratio of 0.07,catalyst mass percentage of 3%in the model fuel,O/S molar ratio of 10∶1,and extractant/oil volume ratio of 1∶1,the desulfurization rate reaches 81.5%by carrying out the PODS reaction under light for 100 min,which is obviously higher than that over CuWO 4;moreover,no obvious decrease of catalytic activity for CuWO4/SBA-15 was observed after 6 runs of PODS.It is proposed that·OH and h+are the main reactive intermediates in PODS.

关 键 词：脱硫 SBA-15 CuWO4 光催化 氧化 

分 类 号：TQ462.1[化学工程—制药化工]