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题名: Self-assembled nanospheres with multiple endohedral binding sites pre-organize catalysts and substrates for highly efficient reactions
作者: Wang, Qi-Qiang1, 3; Gonell, Sergio1; Leenders, Stefan H. A. M.1; Duerr, Maximilian2; Ivanovic-Burmazovic, Ivana2; Reek, Joost N. H.1
刊名: NATURE CHEMISTRY
发表日期: 2016-03-01
卷: 8, 期:3, 页:225-230
收录类别: SCI
英文摘要: Tuning reagent and catalyst concentrations is crucial in the development of efficient catalytic transformations. In enzyme-catalysed reactions the substrate is bound-often by multiple non-covalent interactions-in a well-defined pocket close to the active site of the enzyme; this pre-organization facilitates highly efficient transformations. Here we report an artificial system that co-encapsulates multiple catalysts and substrates within the confined space defined by an M12L24 nanosphere that contains 24 endohedral guanidinium-binding sites. Cooperative binding means that sulfonate guests are bound much more strongly than carboxylates. This difference has been used to fix gold-based catalysts firmly, with the remaining binding sites left to pre-organize substrates. This strategy was applied to a Au(I)-catalysed cyclization of acetylenic acid to enol lactone in which the pre-organization resulted in much higher reaction rates. We also found that the encapsulated sulfonate-containing Au(I) catalysts did not convert neutral (acid) substrates, and so could have potential in the development of substrate-selective catalysis and base-triggered on/off switching of catalysis.
语种: 英语
内容类型: 期刊论文
URI标识: http://ir.iccas.ac.cn/handle/121111/35868
Appears in Collections:分子识别与功能实验室_期刊论文

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作者单位: 1.Univ Amsterdam, Homogeneous Supramol & Bioinspired Catalysis, Vant Hoff Inst Mol Sci, Sci Pk 904, NL-1098 XH Amsterdam, Netherlands
2.Univ Erlangen Nurnberg, Lehrstuhl Bioanorgan Chem, Dept Chem & Pharm, Egerlandstr 3, D-91058 Erlangen, Germany
3.Chinese Acad Sci ICCAS, Inst Chem, CAS Key Lab Mol Recognit & Funct, Beijing 100190, Peoples R China
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