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耐水性共功能化介孔SBA-15的制备及其在甘油与乙酸酯化反应中的应用
引用本文:李瑞云,宋河远,金福祥,陈静.耐水性共功能化介孔SBA-15的制备及其在甘油与乙酸酯化反应中的应用[J].分子催化,2019,33(2):149-158.
作者姓名:李瑞云  宋河远  金福祥  陈静
作者单位:中国科学院兰州化学物理研究所 羰基合成与氧化国家重点实验室, 甘肃 兰州 730000;中国科学院大学, 北京 100049,中国科学院兰州化学物理研究所 羰基合成与氧化国家重点实验室, 甘肃 兰州 730000;中国科学院大学, 北京 100049,中国科学院兰州化学物理研究所 羰基合成与氧化国家重点实验室, 甘肃 兰州 730000;中国科学院大学, 北京 100049,中国科学院兰州化学物理研究所 羰基合成与氧化国家重点实验室, 甘肃 兰州 730000
基金项目:(国家自然科学基金(21673259);江苏省自然科学基金(No.BK20171241))
摘    要:通过后嫁接法合成了一系列耐水性的丙烷磺酸和正辛基共功能化的介孔SBA-15催化剂.采用BET、XRD、FT-IR、TG、TEM及酸碱滴定的方法对催化剂进行了结构性能表征,并将其应用在丙三醇和乙酸的酯化反应中.Octyl-PrSO3H-SBA-15由于较高的酸量以及极好的耐水性而在丙三醇和乙酸酯化反应中取得了100%的丙三醇转化率和89.9%的甘油二乙酸酯和三乙酸酯收率.对影响丙三醇转化率和产物选择性的反应温度、反应时间、催化剂量及反应物比例等进行了讨论.通过向反应体系中加入一定量额外的水对功能化的催化剂的耐水性进行了考察.催化剂Octyl-PrSO3H-SBA-15具有比PrSO3H-SBA-15更好的耐水性能,并且对该催化剂Octyl-PrSO3H-SBA-15在循环使用9次以后,其催化活性基本保持不变.

关 键 词:介孔材料  丙烷磺酸  正辛基基团  共功能化  耐水性
收稿时间:2019/3/18 0:00:00
修稿时间:2019/3/30 0:00:00

Water-tolerant Co-functionalized Mesostructure SBA-15 as Efficient Catalysts for Glycerol-acetic acid Esterification
LI Rui-yun,SONG He-yuan,JIN Fu-xiang and CHEN Jing.Water-tolerant Co-functionalized Mesostructure SBA-15 as Efficient Catalysts for Glycerol-acetic acid Esterification[J].Journal of Molecular Catalysis (China),2019,33(2):149-158.
Authors:LI Rui-yun  SONG He-yuan  JIN Fu-xiang and CHEN Jing
Institution:State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, China;University of Chinese Academy of Sciences, Beijing 100049, China,State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, China;University of Chinese Academy of Sciences, Beijing 100049, China,State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, China;University of Chinese Academy of Sciences, Beijing 100049, China and State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, China
Abstract:A series of water-tolerant propylsulfonic acid and n-octyl group co-functionalized mesostructure SBA-15 were prepared by post-modification. Physico-chemical properties of synthesized catalysts were examined by N2 adsorption-desorption (BET), XRD, FT-IR, TG, TEM and acid-base titration. Catalytic performance was evaluated in the glycerol-acetic acid esterification reaction and effect of reaction temperature, reaction time, catalyst loading, and molar ratio of reactants on conversion and selectivity were investigated. Octyl-PrSO3H-SBA-15 used as catalyst could obtain 100% glycerol conversion and 89.9% diacetin and triacetin selectivity for high acid content and hydrophobicity. Water tolerance of the catalysts were examined by the addition of the increasing amount of water, and Octyl-PrSO3H-SBA-15 exhibited better water tolerance compared to less hydrophobic PrSO3H-SBA-15. Co-functionalized mesoporous catalysts are reusable, with no obvious loss in catalytic activity after nine cycles.
Keywords:mesoporous silica  propylsulfonic acid  n-octyl group  co-functionalization  water tolerance
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