改性SBA-15固载磷钨钼多酸H3PWnMo12-n-O34(n=0,6,12)催化合成柠檬酸三丁酯  

Catalytic synthesis of tributyl citrate with modified SBA-15 supported phospho-tungsten-molybdenum polyacid H3PWnMo12-n-O34(n=0,6,12)

作　　者：王斌 吴克 小梅 刘哲林[2] 徐玲[1] 刘宗瑞[1] WANG Bin;WU Ke;XIAO Mei;LIU Zhe-lin;XU Ling;LIU Zong-rui(College of Chemistry and Materials Science,Inner Mongolia University for the Nationalities,Tongliao 028043,China;School of Chemistry&Environment Engineering,Changchun University of Science and Technology,Changchun 130022,China)

机构地区：[1]内蒙古民族大学化学与材料学院,内蒙古通辽028043 [2]长春理工大学化学与环境工程学院,吉林长春130022

出　　处：《东北师大学报（自然科学版）》2020年第4期98-105,共8页Journal of Northeast Normal University(Natural Science Edition)

基　　金：国家自然科学基金资助项目(21661026);内蒙古自治区自然科学基金资助项目(2019MS02002,2018BS02001);内蒙古自治区高等高校“青年科技英才”支持计划项目(NJYT-18-B22,NJYT-19-B28);内蒙古民族大学科学研究基金资助项目(NMDYB19051);内蒙古民族大学研究生科研创新资助项目(NMDSS1860).

摘　　要：以3-氨丙基三乙氧基硅烷改性的SBA-15为载体,以具有不同组成的Keggin型磷钨钼杂多酸H3PWnMo12-n-O34(n=0,6,12)为固体酸催化剂,通过对SBA-15表面修饰获得一系列介孔分子筛/硅烷偶联剂@磷钨钼杂多酸复合催化剂PWMo@SBA-15/Apts,并利用FTIR、P-XRD、TEM、N2吸附-脱附对复合催化剂的组成、结构及形貌进行了表征.以PWMo@SBA-15/Apts为催化剂对柠檬酸三丁酯的催化合成进行研究,考察不同多酸组成、催化剂用量、酸醇物质的量比、反应时间、反应温度对催化合成柠檬酸三丁酯酯化率的影响.结果表明:固载磷钨酸催化剂合成柠檬酸三丁酯的酯化率最高可达97.36%,重复使用8次后酯化率仍可达74.38%.A series of mesoporous molecular sieves/silane coupling agent@phosphotungstic-molybdium acid composite catalysts PWMo@SBA-15/Apts were prepared through surface modification of SBA-15,when the 3-aminopropyltriethoxysilane modified SBA-15 was used as carrier and the Keggin type phosphotungsticmolybdium acid with different composition H3PWnMo12-n-O34(n=0,6,12)were used as solid acid catalysts.The composition,structure and morphology of the composite catalysts were characterized by FTIR,P-XRD,TEM and N2 adsorption-desorption.The catalytic synthesis of tributyl citrate was studied with PWMo@SBA-15/Apts as catalysts.The effects of composition of polyacid,amount of catalyst,molar ratio of acid to alcohol,reaction time and reaction temperature on the esterification rate of tributyl citrate were studied.The results showed that the highest esterification rate of tributyl citrate was 97.36%catalyzed by supported phosphotungstic acid catalyst,and the esterification rate was still 74.38%after 8 times of recycling.

关 键 词：杂多酸 介孔分子筛 催化化学 柠檬酸三丁酯 

分 类 号：O611[理学—无机化学]