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介孔多金属氧酸盐基离子杂化物作为一种三相催化剂用于在水相中用H₂O₂氧化苯甲醇。

Mesoporous polyoxometalate-based ionic hybrid as a triphasic catalyst for oxidation of benzyl alcohol with H(2)O(2) on water.

作者信息

Chen Guojian, Zhou Yu, Long Zhouyang, Wang Xiaochen, Li Jing, Wang Jun

机构信息

State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemistry and Chemical Engineering, Nanjing Tech University , Nanjing 210009, PR China.

出版信息

ACS Appl Mater Interfaces. 2014 Mar 26;6(6):4438-46. doi: 10.1021/am5001757. Epub 2014 Mar 14.

Abstract

A self-assembled mesoporous polyoxometalate-based ionic hybrid catalyst [TMGHA]2.4H0.6PW was prepared by combination of alcohol amino-tethered guanidinium ionic liquid [TMGHA]Cl with Keggin phosphotungstic acid H3PW12O40 (PW). Nitrogen sorption experiment validated the formation of mesostructure with moderate BET surface area, and scanning and transmission electron microscopy (SEM and TEM) showed a fluffy coral-shaped morphology for the hybrid. The contact angle test displayed that the hybrid owned hydrophilic-hydrophobic balanced surface that exhibited well wettability for both water and organic substrate like benzyl alcohol. Therefore, the hybrid can efficiently catalyze the water-mediated triphasic oxidation of benzyl alcohol with H2O2. During the reaction, the triphase catalytic system showed a special "on water" effect mainly due to the suitable mesostructure and surface wettability, thus providing some clues for the preparation of green heterogeneous catalyst.

摘要

通过将醇胺连接的胍离子液体[TMGHA]Cl与Keggin型磷钨酸H3PW12O40(PW)相结合,制备了一种自组装的介孔多金属氧酸盐基离子杂化催化剂[TMGHA]2.4H0.6PW。氮吸附实验验证了具有适度BET表面积的介孔结构的形成,扫描电子显微镜和透射电子显微镜(SEM和TEM)显示该杂化物具有蓬松的珊瑚状形态。接触角测试表明,该杂化物具有亲水-疏水平衡表面,对水和有机底物如苯甲醇均表现出良好的润湿性。因此,该杂化物能够有效地催化以H2O2为氧化剂的水相介导的苯甲醇三相氧化反应。在反应过程中,三相催化体系表现出特殊的“水相上”效应,这主要归因于合适的介孔结构和表面润湿性,从而为绿色多相催化剂的制备提供了一些线索。

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