Wang QQ, Gonell S, Leenders SH, Dürr M, Ivanovic-Burmazovic I, Reek JN (2016)
Publication Status: Published
Publication Type: Journal article
Publication year: 2016
Book Volume: 8
Pages Range: 225-30
Journal Issue: 3
DOI: 10.1038/nchem.2425
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.
APA:
Wang, Q.-Q., Gonell, S., Leenders, S.H., Dürr, M., Ivanovic-Burmazovic, I., & Reek, J.N. (2016). Self-assembled nanospheres with multiple endohedral binding sites pre-organize catalysts and substrates for highly efficient reactions. Nature Chemistry, 8(3), 225-30. https://dx.doi.org/10.1038/nchem.2425
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): 225-30.
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