配体功能化负载型磷钼酸催化剂的制备及其氧化脱硫性能研究  

Preparation of ligand-functionalized supported phosphomolybdic acid and catalytic performance in oxidative desulfurization

作　　者：高爽[1] 葛登文 于悦 张今红 肖舒宁 陈晓陆[1] GAO Shuang;GE Deng-wen;YU Yue;ZHANG Jin-hong;XIAO Shu-ning;CHEN Xiao-lu(Liaoning Provincial Key Laboratory for Synthesis and Separation of Chemical Additives,College of Chemistry and Environmental Engineering,Yingkou Institute of Technology,Yingkou 115014,China)

机构地区：[1]营口理工学院化学与环境工程学院,辽宁省化学助剂合成与分离重点实验室,辽宁营口115014

出　　处：《现代化工》2022年第1期121-126,131,共7页Modern Chemical Industry

基　　金：辽宁省化学助剂合成与分离重点实验室项目(ZJNK2013);辽宁省区域创新联合基金(2020-YKLH-36);营口理工学院2021年大创项目(202114435003)。

摘　　要：以有机配体功能化的SBA-15为载体,将Co取代的磷钼酸(Co-POM)负载于功能化SBA-15载体上制备负载型催化剂。利用XRD、FT-IR、BET、TEM、TG等对催化剂结构进行表征。结果表明,—octyl、—NH_(2)基团成功嫁接到载体SBA-15上;催化剂的整体结构没有发生明显改变,催化剂活性组分均匀地分散在介孔SBA-15的表面和孔道中。以二苯并噻吩(DBT)为底物进行氧化脱硫反应,考察催化剂结构对催化活性的影响。结果表明,—octyl和—NH_(2)基团双功能化的催化剂(CO-POM-octyl-NH_(2)-SBA-15)脱硫效果最好,在反应温度为60℃、负载量为30%、反应时间为8 h、剂油体积比为1∶1的最佳反应条件下,催化剂对DBT脱除率达到94.95%。循环使用5次后,催化性能没有明显降低,具有良好的循环稳定性。A supported catalyst is prepared through supporting Co-modified phosphomolybdic acid(Co-POM) on organic ligands functionalized SBA-15.The catalyst is characterized by XRD,FT-IR,BET,TEM and TG.FT-IR characterization shows that —octyl and —NH_(2) functional groups are successfully grafted onto the surface of SBA-15.XRD,TEM and BET characterization shows that the overall structure of the catalyst does not change significantly, and the active components of the catalyst disperse uniformly in the surface and pore channels of mesoporous SBA-15.Taking the removal of dibenzothiophene(DBT) from simulated oil as the probe reaction, the influence of catalyst structure is evaluated, and the technological conditions of the reaction are optimized.It is found that the catalyst(Co-POM-octyl-NH_(2)-SBA-15) with —octyl and —NH_(2) functional groups has the best desulfurization effect, under the optimum conditions that reaction temperature is at 60℃,the loading amount is 30%,reaction time is 8 h and the volume ratio of oxidant/oil is 1∶1.Under these conditions, the removal rate of DBT by the catalyst achieves 94.95%.No obvious attenuation of catalytic activity for Co-POM-NH_(2)-SBA-15 is observed after 6 runs of oxidative desulfurization, showing a good cyclic stability.

关 键 词：有机配体 氧化脱硫 SBA-15 磷钼酸 二苯并噻吩 

分 类 号：O643.3[理学—物理化学]