Studies on hydrolysis mechanism of anticancer ruthenium drug ImH[trans-Ru(Im)₂Cl₄] via ABEEMσπ polarizable force field combined with QM and MD-FEP

Abstract

We used ABEEMσπ(atom-bond electronegativity equalization method) polarizable force field(ABEEMσπ PFF) method combined with QM and molecular dynamics-free energy perturbation(MD-FEP) methods to investigate the function of water molecules in hydrolysis process of ImH[trans-Ru(Im)₂Cl₄](ICR). The activation free energies obtained via MD-FEP calculation are in fair agreement with the experimental data. In addition, QM/MM(ABEEM) rationally describes the charge distributions and the electrostatic interaction between molecules. ABEEMσπ fluctuating charge model has the following good characteristics: (1) not only atomic charge regions but also σ, π bond and lone pair charge regions are explicitly represented for a molecule; (2) the region charges are geometry dependent and calculated from time to time in the dynamic simulation without any iterative procedure so that its performance is time-saving compared with the Drude model and induced dipole model.

Keywords

Atom-bond electronegativity equalization method(ABEEMσπ) polarizable force field / Quantum mechanics/molecular mechanics(QM/MM) / Molecular dynamics-free energy perturbation / Hydrolysis mechanism / Activation free energy

References

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