Porous metal-metalloporphyrin gel as catalytic binding pocket for highly efficient synergistic catalysis

• Published in: Nature communications Vol. 10; no. 1; p. 1913
• Main Authors: Zhang, Weijie, Dynes, James J., Hu, Yongfeng, Jiang, Pingping, Ma, Shengqian
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 23.04.2019; Nature Publishing Group; Nature Portfolio
• Subjects: 639/638/77/883; 639/638/77/887; 639/638/911/406/910; Aerogels; Binding; Catalysis; Catalysts; Enzymes; Flexibility; Humanities and Social Sciences; multidisciplinary; NMR; Nuclear magnetic resonance; Performance enhancement; Porosity; Recognition; Science; Science (multidisciplinary); Selectivity; Stereoselectivity; Substrates; X ray absorption
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-019-09881-9

Synergistic catalysis occurring in an enzyme pocket shows enhanced performance through supramolecular recognition and flexibility. This study presents an aerogel capable of similar function by fabricating a gel catalyst with hierarchical porosity. Here, the as-prepared Co-MMPG, a Co(II) metal-metalloporphyrin gel, maintains enough conformational flexibility and features a binding pocket formed from the co-facial arrangement of the porphyrin rings, as elucidated through the combined studies of solid-state NMR and X-ray absorption near-edge structure (XANES). The cooperativity between two Co(II) sites within the defined nanospace pocket facilitates the binding of different substrates with a favourable geometry thereby rendering Co-MMPG with excellent performance in the context of synergistic catalysis, especially for the kinetic control stereoselective reactions. Our work thus contributes a different enzyme-mimic design strategy to develop a highly efficient heterogeneous catalyst with high chemo/stereo selectivity. Synergistic catalysis occurring in an enzyme pocket shows enhanced performance through supramolecular recognition and flexibility. Here the authors design an enzyme-mimic strategy to develop a Co(II) metal-metalloporphyrin gel with excellent synergistically catalytic performance and chemo/stereo selectivity.