双酸位SO42-/ZrO2-SiO2固载离子液体催化剂的构筑及性能
Construction and Properties of SO42-/ZrO2-SiO2 Immobilized Ionic Liquid Catalysts with Double-Acid Active Sites
作者单位E-mail
范明明 江南大学化学与材料工程学院, 食品胶体与生物技术教育部重点实验室, 无锡 214122  
刘慧 江南大学化学与材料工程学院, 食品胶体与生物技术教育部重点实验室, 无锡 214122  
倪邦庆 江南大学化学与材料工程学院, 食品胶体与生物技术教育部重点实验室, 无锡 214122 ni1221ni@126.com 
张萍波 江南大学化学与材料工程学院, 食品胶体与生物技术教育部重点实验室, 无锡 214122 pingbozhang@126.com 
摘要: 采用一步共缩合-水热法合成酸性载体SO42-/ZrO2-SiO2,化学法接枝酸性离子液体磺酸功能化咪唑硫酸氢盐([Ps-im]HSO4),构筑拥有Brönsted与Lewis双酸位的离子液体固载型催化剂SO42-/ZrO2-SiO2-IL。采用X射线衍射、傅里叶红外、N2吸附-脱附、X射线光电子能谱、热重以及透射电镜对催化剂的结构进行表征,结果表明:锆原子和酸性结构SO42-被成功引入纯硅材料,所合成的载体具有一定酸性;离子液体成功固载于酸性介孔材料SO42-/ZrO2-SiO2,且固载后的催化剂保持其介孔结构。以大豆油和甲醇的酯交换反应为探针,考察了SO42-/ZrO2-SiO2-IL催化剂的催化性能。在反应温度为150℃、反应时间为4 h、催化剂量5%(w/w)、醇油物质的量之比为24:1的反应条件下,生物柴油的收率超过92%,且回收利用5次后,生物柴油的收率仍达86%。
关键词: 双酸位  生物柴油  酸性介孔材料  离子液体  固载
基金项目: 国家自然科学基金(No.21306063)资助项目。
Abstract: The immobilized catalyst SO42-/ZrO2-SiO2-IL with double-acid active sites,namely Brönsted and Lewis acid sites,was synthesized by immobilization of acid ionic liquid sulfonic acid functionalized imidazolium hydrogen sulfate ([Ps-im]HSO4) onto the surface of the acidic mesoporous material SO42-/ZrO2-SiO2 which was prepared by a one-step co-condensation technique combined with hydrothermal treatment.The structure of the catalyst was characterized by XRD,FT-IR,N2 absorption-desorption measurement,XPS,thermogravimetric analysis and TEM.The results showed that zirconium and acid structure (SO42-) were incorporated into the framework of pure silicon,bringing a certain acidity;and it also demonstrated that the ionic liquid was successfully immobilized onto the acidic mesoporous materials SO42-/ZrO2-SiO2 and the structure of the catalyst remained intact.The activity of SO42-/ZrO2-SiO2-IL was investigated by the transesterification of soybean oil with methanol for biodiesel production as the probe reaction.The yield of biodiesel was more than 92% when the reaction was carried out under the following condition:reaction temperature,150℃;reaction time,4 h;amount of catalyst,5%(w/w);methanol to soybean oil,24:1.And the catalyst still yielded about 86% after five cycles.
Keywords: double-acid active sites  biodiesel  acidic mesoporous material  ionic liquid  immobilize
投稿时间:2016-08-09 修订日期:2016-11-01
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