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A Chemically Fuelled Molecular Automaton Displaying Programmed Migration of Zn(2+) Between Alternative Binding Sites

A molecular system comprising a cationic zinc complex and an amino acid‐derived ambident ligand having phosphate and carboxylate binding sites undergoes a series of rearrangements in which the metal cation migrates autonomously from one site to another. The location of the metal is identified by the...

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Detalles Bibliográficos
Autores principales: Wootten, Matthew M., Tshepelevitsh, Sofja, Leito, Ivo, Clayden, Jonathan
Formato: Online Artículo Texto
Lenguaje:English
Publicado: John Wiley and Sons Inc. 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9804598/
https://www.ncbi.nlm.nih.gov/pubmed/35880579
http://dx.doi.org/10.1002/chem.202202247
Descripción
Sumario:A molecular system comprising a cationic zinc complex and an amino acid‐derived ambident ligand having phosphate and carboxylate binding sites undergoes a series of rearrangements in which the metal cation migrates autonomously from one site to another. The location of the metal is identified by the circular dichroism spectrum of a ligated bis(2‐quinolylmethyl)‐(2‐pyridylmethyl)amine (BQPA) chromophore, which takes a characteristic shape at each binding site. Migration is fuelled by the decomposition of trichloroacetic acid to CO(2) and CHCl(3), which progressively neutralises the acidity of the system as a function of time, revealing in sequence binding sites of increasing basicity. The migration rate responds to control by variation of the temperature, water content and triethylamine concentration, while an excess of fuel controls the duration of an induction period before the migration event.