功能化离子液体嵌入SBA-15负载磷钨酸催化剂制备及其催化性能.doc

功能化离子液体嵌入SBA-15负载磷钨酸催化剂制备摘 要：一种新型的双咪唑离子液体功能化采用共水解-缩聚一步了有机-无机杂化介孔材料 (PMO-SBA-15)，中嵌入的离子液体为稳定剂，采用离子交换制备了PMO-SBA-15的磷钨酸催化剂 (PW-IL-PMO-SBA-15)。SBA-15材料依然保持原材料的有序六方孔道结构；PW在材料的孔道内壁均匀分布，而且维持原有的Keggin 结构。以苯甲醇选择催化剂中离子液体的嵌入含量和磷钨酸的负载量，苯甲醇的转化率和苯甲醛的选择性分别95.4 % 和94 %磷钨酸PW-IL-PMO-SBA-15催化剂在该反应中可重复使用。 关键词：有机-无机杂化介孔材料; 离子液体; 磷钨酸; ; 氧化 The Preparation and Catalytic Performances of SBA-15 Embeded Functional Ionic Liquid for Loading Phosphowolframic Acid Abstract: The preparation of a novel periodic mesoporous organosilica of SBA-15 functionalized by ionic liquid to load phosphowolframic acid (PW) was used as a catalyst in the oxidation of benzyl alcohol. The mesoporous organosilica (PMO-SBA-15) was synthesized via a one-pot condensation process involving the assembly of triethylenetetramine silsesquioxane organic precursor containing amine group and tetraethoxysilane (TEOS) in the presence of P123 (EO20PO70EO20). Phosphowolframic acid was grafted by ionic liquid to obtain PW-containing mesoporous organosilica (PW-IL-PMO-SBA-15) with ion-exchange. The resultant materials were characterized by XRD and TEM, and the results indicated that the PW were well dispersed uniformly inside into the channel of the PMO-SBA-15 with retaining its Keggin structure. The effects of the content of ionic liquid moieties and phosphowolframic acid loading in the catalyst of PW-IL-PMO-SBA-15 on the oxidation of benzyl alcohol were investigated. The PW-IL-PMO- SBA-15 exhibited high catalytic activity and reusability. The conversion of benzyl alcohol and the selectivity for benzaldehyde were as high as 95.4% and 94%, respectively, when the reaction was performed at100 oC for 6 h using hydrogen peroxide as the oxidant and water as the solvent. Keywords: periodic mesoporous organosilicas; ionic liquid; phosphowolframic acid; benzyl alcohol; oxidation 1前言 醇类化合物催化氧化羰基化合物是有机中间体合成中的重要反应[1-3]。苯甲醛是精细化工中重要的中间体，广泛用于染料、医药、农药、食品和香料等的工业生产中[4]。其合成可从不同的原料经过不同的途径实现多年来工业上生产苯甲醛大多采用甲苯直接氧化法和甲苯侧链氯化后水解法，然而这些方法工艺复杂，要求用到化学计量比催化剂和氧化剂，