磷钨酸改性TS-1催化剂的制备及其催化油酸甲酯环氧化反应性能  

Preparation of phosphotungstic acid-modified TS-1 catalyst and its catalytic performance for methyl oleate epoxidation

作　　者：周凯 张颖琦 骆贝宁 何文清 颜贤仔[1] 吴国强[1] ZHOU Kai;ZHANG Yingqi;LUO Beining;HE Wenqing;YAN Xianzai;WU Guoqiang(School of Food Science and Engineering,Jiangxi Agricultural University,Nanchang 330045,China)

机构地区：[1]江西农业大学食品科学与工程学院,江西南昌330045

出　　处：《石油化工》2024年第12期1712-1719,共8页Petrochemical Technology

基　　金：国家自然科学基金项目(21802055);江西省自然科学基金杰出青年基金项目(20242BAB23071);江西省自然科学基金面上项目(20202BABL205013)。

摘　　要：采用传统水热法合成了钛硅沸石(TS-1),再用磷钨酸(HPA)对TS-1改性制备了HPA/TS-1催化剂,并将催化剂用于油酸甲酯(MO)环氧化反应中。利用XRD、FTIR、N_(2)吸附-脱附、UV-Vis、SEM、TEM等方法对催化剂的结构进行表征,考察了HPA/TS-1催化剂在MO环氧化反应中的催化性能。实验结果表明,HPA被均匀地分散在TS-1表面,未破坏TS-1的晶型结构和四配位Ti的配位状态。6%HPA/TS-1催化剂展现出较高的催化活性,MO转化率为81.35%。6%HPA/TS-1催化MO环氧化反应的最佳工艺条件为:反应温度80℃、反应时间12 h、6%HPA/TS-10.1 g、n(MO)∶n(H_(2)O_(2))=1∶3。催化剂重复使用3次后,MO转化率从45.25%降至28.76%,经过170℃再生后催化剂活性得到较大的恢复。Titanium silicalite zeolite(TS-1)was synthesized by the traditional hydrothermal method,and TS-1 was modified by phosphotungstic acid(HPA)to prepare catalysts(HPA/TS-1),which was used in the epoxidation of methyl oleate(MO).The structure of the catalysts was systematically characterized by XRD,FTIR,N_(2)adsorption-desorption,UV-Vis,SEM,TEM,etc.,and the catalytic performance of the HPA/TS-1 catalysts was also investigated in the epoxidation of MO.The results show that the HPA is uniformly dispersed on the surface of TS-1 zeolite and does not destroy the crystal framework structure of TS-1 and the coordination state of tetrahedrally coordinated Ti.Furthermore,the 6%HPA/TS-1 catalyst exhibits higher catalytic activity,suggesting that the MO conversion is 81.35%.The optimal epoxidation process catalyzed by 6%HPA/TS-1 is the reaction temperature of 80℃,reaction time of 12 h,catalyst dosage of 0.1 g,and n(MO)∶n(H_(2)O_(2))of 1∶3.Additionally,the MO conversion decreases from 45.25%to 28.76%after three times of catalyst reuse,but the catalyst activity is significantly restored through the regeneration at 170℃.

关 键 词：钛硅沸石 磷钨酸 油酸甲酯 环氧化 骨架钛 酸性 

分 类 号：TQ414[化学工程]