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Simulating the Chelate Effect

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    Simulating the Chelate Effect
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2018, 140, 45, 15166–15169
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    https://doi.org/10.1021/jacs.8b09371
    Published November 1, 2018
    Copyright © 2018 American Chemical Society
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    Abstract

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    Despite the rich history of experimental studies focusing on the thermochemistry and kinetics associated with the chelate effect, molecular-level computational studies on the chelate ring opening/ring closure are scarce. The challenge lies in an accurate description of both the metal ion and its aqueous environment. Herein, we demonstrate that an optimized 12-6-4 Lennard-Jones (LJ) model can capture the thermodynamics and provide detailed structural and mechanistic insights into the formation of ethylenediamine (en) complexes with metal ions. The water molecules in the first solvation shell of the metal ion are found to facilitate the chelate ring formation. The optimized parameters further simulate the formation of bis and tris(en) complexes representing the wide applicability of the model to simulate coordination chemistry and self-assembly processes.

    Copyright © 2018 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/jacs.8b09371.

    • Details of the simulation protocols, parameter fitting, computed binding free energies for different divalent ions and en for m12-6-4 ion model (PDF)

    • Video showing reaction profile of metal ligand association (AVI)

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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2018, 140, 45, 15166–15169
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.8b09371
    Published November 1, 2018
    Copyright © 2018 American Chemical Society
    Request reuse permissions

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