Self-assembled nanospheres with multiple endohedral binding sites pre-organize catalysts and substrates for highly efficient reactions
文献类型：期刊论文
| 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
 |
| 出版日期 | 2016-03-01 |
| 卷号 | 8期号:3页码:225-230 |
| 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. |
| 收录类别 | SCI |
| 语种 | 英语 |
| 源URL | [http://ir.iccas.ac.cn/handle/121111/35868]  |
| 专题 | 化学研究所_分子识别与功能实验室 |
| 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 |
| 推荐引用方式 GB/T 7714 | Wang, Qi-Qiang,Gonell, Sergio,Leenders, Stefan H. A. M.,et al. Self-assembled nanospheres with multiple endohedral binding sites pre-organize catalysts and substrates for highly efficient reactions[J]. NATURE CHEMISTRY,2016,8(3):225-230. |
| APA | Wang, Qi-Qiang,Gonell, Sergio,Leenders, Stefan H. A. M.,Duerr, Maximilian,Ivanovic-Burmazovic, Ivana,&Reek, Joost N. H..(2016).Self-assembled nanospheres with multiple endohedral binding sites pre-organize catalysts and substrates for highly efficient reactions.NATURE CHEMISTRY,8(3),225-230. |
| MLA | Wang, Qi-Qiang,et al."Self-assembled nanospheres with multiple endohedral binding sites pre-organize catalysts and substrates for highly efficient reactions".NATURE CHEMISTRY 8.3(2016):225-230. |
入库方式： OAI收割
来源：化学研究所
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