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- W3185014724 abstract "Abstract In this study, the ligand exchange mechanism at a biomimetic Zn II centre, embedded in a pocket mimicking the possible constrains induced by a proteic structure, is explored. The residence time of different guest ligands (dimethylformamide, acetonitrile and ethanol) inside the cavity of a calix[6]arene‐based tris(imidazole) tetrahedral zinc complex was probed using 1D EXchange SpectroscopY NMR experiments. A strong dependence of residence time on water content was observed with no exchange occurring under anhydrous conditions, even in the presence of a large excess of guest ligand. These results advocate for an associative exchange mechanism involving the transient exo‐coordination of a water molecule, giving rise to 5‐coordinate Zn II intermediates, and inversion of the pyramid at the Zn II centre. Theoretical modelling by DFT confirmed that the associative mechanism is at stake. These results are particularly relevant in the context of the understanding of kinetic stability/lability in Zn proteins and highlight the key role that a single water molecule can play in catalysing ligand exchange and controlling the lability of Zn II in proteins." @default.
- W3185014724 created "2021-08-02" @default.
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- W3185014724 date "2021-08-11" @default.
- W3185014724 modified "2023-10-03" @default.
- W3185014724 title "A Water Molecule Triggers Guest Exchange at a Mono‐Zinc Centre Confined in a Biomimetic Calixarene Pocket: a Model for Understanding Ligand Stability in Zn Proteins" @default.
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- W3185014724 doi "https://doi.org/10.1002/chem.202102184" @default.
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