新型多酸-有机亚胺-分子筛杂化材料的氧化催化性能  

Oxidation catalytic activity of novel SiNiW_(11)-Schiff-SBA-15 hybrid materials

作　　者：胡江磊[1] 冯文平[1] 郭伊荇[2] 张龙[1] 

机构地区：[1]长春工业大学化工学院,吉林长春130012 [2]东北师范大学化学学院,吉林长春130024

出　　处：《化工学报》2011年第6期1563-1568,共6页CIESC Journal

基　　金：国家自然科学基金项目(20873018);吉林省科技厅科学研究项目(20080312)

摘　　要：利用3-氨基丙基三甲氧基硅修饰的SBA-15、苯甲醛以及过渡金属单取代Keggin型杂多酸盐(SiNiW11)合成了一系列有序介孔二氧化硅杂化材料(SiNiW11-Schiff-SBA-15)。通过对杂化材料进行表征,证明SiNiW11的Keggin单元以及希夫碱配体在负载之后结构保持完整,并研究了杂化材料的形貌和表面物理化学性质。制备的杂化催化剂的氧化催化性能通过过氧化氢选择性氧化苯乙烯反应进行系统研究。在乙腈溶剂中,使用100 mg催化剂,H2O2与苯乙烯的摩尔比为1∶1,60℃条件下反应12 h,苯乙烯的转化率为56.8%,苯甲醛的选择性可达到97.0%。最后,对杂化催化剂的循环使用情况进行了评价。A series of ordered mesoporous silica hybrid materials（SiNiW11-Schiff-SBA-15）were prepared by using successive grafting procedures of SBA-15 silica with 3-aminopropyl-trimethoxysilane,benzaldehyde,and transition metal-monosubstituted Keggin-type polyoxometalates（SiNiW11）.The hybrid materials were characterized to confirm the structure integrity of the Keggin unit and Schiff base ligand after the incorporation and to investigate the morphology and surface textural properties of the composite catalysts.These materials were subsequently utilized as efficient and selective catalysts in the reaction of oxidation of styrene to benzaldehyde using H2O2 as an oxidant.The conversion of styrene and the selectivity to benzaldehyde were 56.8% and 97.0%,under the condition of acetonitrile media,100 mg catalyst,1∶1 H2O2 to styrene molar ratio,and reaction at 60℃ for 12 h.Finally,the reusability of the catalysts was evaluated.

关 键 词：有序介孔材料 杂多酸盐 希夫碱 选择性氧化 苯甲醛 

分 类 号：TQ01[化学工程]