Tuning the adsorption interactions of imidazole derivatives with specific metal cations.
In this work, we report a computational study of the interactions between metal cations and imidazole derivatives in the gas phase. We first performed a systematic assessment of various density functionals and basis sets for predicting the binding energies between metal cations and the imidazoles. We find that the M11L functional in combination with the 6-311++G(d,p) basis set provides the best compromise between accuracy and computational cost with our metal···imidazole complexes. We then evaluated the binding of a series of metal cations, including Li(+), Na(+), K(+), Co(2+), Ni(2+), Cu(2+), Zn(2+), Cd(2+), Ba(2+), Hg(2+), and Pb(2+), with several substituted imidazole derivatives. We find that electron-donating groups increase the metal-binding energy, whereas electron-withdrawing groups decrease the metal-binding energy. Furthermore, the binding energy trends can be rationalized by the hardness of the metal cations and imidazole derivatives, providing a quick way to estimate the metal···imidazole binding strength. This insight can enable efficient screening protocols for identifying effective imidazole-based solvents and membranes for metal adsorption and provide a framework for understanding metal···imidazole interactions in biological systems.
Department of Chemical and Biological Engineering, The University of Alabama , Box 870203, Tuscaloosa, Alabama 35487-0203, United States.
Haining
H
Liu
Jason E
JE
Bara
C Heath
CH
Turner
D000327:Adsorption; D002412:Cations / Q000737:chemistry*; D003198:Computer Simulation; D004583:Electrons; D004791:Enzyme Inhibitors / Q000737:chemistry*; D007093:Imidazoles / Q000737:chemistry*; D008670:Metals / Q000737:chemistry*; D008956:Models, Chemical; D015394:Molecular Structure
D002412:Cations; D004791:Enzyme Inhibitors; D007093:Imidazoles; D008670:Metals; C029899:imidazole