Spatial Coordination of Cooperativity in Silica-Supported Cu/TEMPO/Imidazole Catalytic Triad

被引：37

作者：

Chandra, Prakash ^{[1
]}

Jonas, Alain M. ^{[1
]}

Fernandes, Antony E. ^{[1
]}

机构：

[1] Catholic Univ Louvain, Inst Condensed Matter & Nanosci, B-1348 Louvain La Neuve, Belgium

来源：

ACS CATALYSIS | 2018年 / 8卷 / 07期

关键词：

supported catalysis; multifunctional catalysts; cooperativity; CuAAC; alcohol oxidation; HETEROGENEOUS SYNERGISTIC CATALYSIS; TSUJI-TROST REACTION; MESOPOROUS SILICA; AEROBIC OXIDATION; ALCOHOL OXIDATION; FUNCTIONAL-GROUPS; CONCERTED CATALYSIS; ALDOL CONDENSATION; PALLADIUM COMPLEX; HYBRID MATERIALS;

D O I：

10.1021/acscatal.8b01399

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Multifunctional catalysts obtained by the covalent immobilization of discrete molecular species on porous supports represent a unique approach to emulate some of the design principle and performances of enzymes. However, it is decisive in such systems to control the stoichiometry, spatial distribution, and proximity between the grafted catalytic centers to satisfy the chemical and geometrical requirements for cooperativity. Here, we present strategies to optimize the activity of a catalytic triad on mesoporous silica particles in the representative aerobic oxidation of benzyl alcohol and show that, in contrast with the more-traditional mixed-monolayer approach, activity can be amplified by tuning the spatial distribution of the co-catalysts to maximize the probability of full synergistic pairings.

引用

页码：6006 / 6011

页数：11

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