A Theoretical Study on the Hydrolysis Process of the Antimetastatic Ruthenium(III) Complex NAMI-A
详细信息 查看全文
- 作者：Jincan Chen ; Lanmei Chen ; Siyan Liao ; Kangcheng Zheng ; Liangnian Ji
- 刊名：Journal of Physical Chemistry B
- 出版年：2007
- 出版时间：July 12, 2007
- 年：2007
- 卷：111
- 期：27
- 页码：7862 - 7869
- 全文大小：294K
- 年卷期：v.111,no.27(July 12, 2007)
- ISSN：1520-5207
文摘
A hydrolysis process of the anticancer drug ImH[trans-Ru(III)Cl4(DMSO)(Im)] (nicknamed NAMI-A; Im =imidazole, DMSO = dimethyl sulfoxide) has been studied by using density functional theory (DFT) method,and the aqueous solution effect has been considered and calculated by conductor-like polarizable calculationmodel (CPCM). The stationary points on the potential energy surfaces for the first and second hydrolysissteps (including two different paths) were fully optimized and characterized. The following was found: forthe first hydrolysis process, the computed relative free energies 
G
(aq) and rate constant (k) in aqueoussolution are 23.2 kcal/mol and 6.11 × 10-5 s-1, respectively, in satisfactory agreement with the experimentalvalues; for the second hydrolysis step, some disagreement still exists, and thus more accurate solvent modelneeds to be designed and improved. On the basis of our present limited work, it can reasonably suggest thatthe hydrolysis process of NAMI-A perform mainly via the first hydrolysis step and then the path 1 of thesecond hydrolysis step. The theoretical results provide the structural properties as well as the detailed energyprofiles for the mechanism of hydrolysis of NAMI-A, such results may assist in understanding the reactionmechanism of the anticancer drug with the biomolecular target.
G (aq) and rate constant (k) in aqueoussolution are 23.2 kcal/mol and 6.11 × 10-5 s-1, respectively, in satisfactory agreement with the experimentalvalues; for the second hydrolysis step, some disagreement still exists, and thus more accurate solvent modelneeds to be designed and improved. On the basis of our present limited work, it can reasonably suggest thatthe hydrolysis process of NAMI-A perform mainly via the first hydrolysis step and then the path 1 of thesecond hydrolysis step. The theoretical results provide the structural properties as well as the detailed energyprofiles for the mechanism of hydrolysis of NAMI-A, such results may assist in understanding the reactionmechanism of the anticancer drug with the biomolecular target.