Knowledge Management System Of Guangzhou Institute of Energy Conversion, CAS
Mechanism of aquation and nucleobase binding of ruthenium (II) and osmium (II) arene complexes: A systematic comparison DFT study | |
Wang, Hanlu1; DeYonker, Nathan J.2; Gao, Hui3; Ji, Liangnian1; Zhao, Cunyuan1; Mao, Zong-Wan1 | |
2012-05-01 | |
发表期刊 | JOURNAL OF ORGANOMETALLIC CHEMISTRY
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卷号 | 704页码:17-28 |
摘要 | A systematic mechanistic study is reported for the aquation and nucleobase binding process of a series of Ru-II and Os-II arene-based anticancer drug complexes using density functional theory and COSMO implicit solvent model. The structures of Ru-II and Os-II complexes are similar to each other because of lanthanide contraction of osmium. However, the aquation was substantially more facile for Ru-II complexes than Os-II complexes. As to nucleobase substitution, various possible paths were explored based on considering the initial conformation of ethylenediamine (en) and the orientation of guanine (G) and adenine (A). Both Ru and Os complexes exhibited much lower free energy barrier for G than A. This observed predominance toward G mainly originated from larger stabilization energy for the initially formed complex, compared with A, in combination with favored kinetics and thermodynamics. Moreover, the calculations indicated that pK(a)s of Os-bound water molecules were uniformly much lower than those of Ru-bound water molecules. Analysis of the natural bond orbital (NBO) charge reveals that Os-II has a higher net positive charge than Ru-II, leading to a stronger electrostatic attractive interaction between Os-II and chloride or water, resulted in higher activation barrier for their departure. These differences between Ru-II and Os-II en complexes discussed in our study may partly explain the inertness of the Os-II complexes in biological system. (C) 2012 Elsevier B.V. All rights reserved. |
文章类型 | Article |
关键词 | Dft Ruthenium Osmium Aquation Nucleobase Pk(a) |
WOS标题词 | Science & Technology ; Physical Sciences |
DOI | 10.1016/j.jorganchem.2011.12.034 |
研究领域[WOS] | Chemistry |
关键词[WOS] | EFFECTIVE CORE POTENTIALS ; CANCER-CELL CYTOTOXICITY ; ANTICANCER COMPLEXES ; ORGANOMETALLIC RUTHENIUM(II) ; MOLECULAR CALCULATIONS ; DNA-BINDING ; ANTITUMOR COMPLEXES ; CISPLATIN BINDING ; SOLVATION METHODS ; OVARIAN-CANCER |
收录类别 | SCI |
语种 | 英语 |
WOS类目 | Chemistry, Inorganic & Nuclear ; Chemistry, Organic |
WOS记录号 | WOS:000300638400003 |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://ir.giec.ac.cn/handle/344007/10181 |
专题 | 中国科学院广州能源研究所 |
作者单位 | 1.Sun Yat Sen Univ, Sch Chem & Chem Engn, KLGHEI Environm & Energy Chem, MOE Key Lab Bioinorgan & Synthet Chem, Guangzhou 510275, Guangdong, Peoples R China 2.Univ Memphis, Dept Chem, Memphis, TN 38152 USA 3.Chinese Acad Sci, Guangzhou Inst Energy Convers, Key Lab Renewable Energy & Gas Hydrate, Guangzhou 510640, Guangdong, Peoples R China |
推荐引用方式 GB/T 7714 | Wang, Hanlu,DeYonker, Nathan J.,Gao, Hui,et al. Mechanism of aquation and nucleobase binding of ruthenium (II) and osmium (II) arene complexes: A systematic comparison DFT study[J]. JOURNAL OF ORGANOMETALLIC CHEMISTRY,2012,704:17-28. |
APA | Wang, Hanlu,DeYonker, Nathan J.,Gao, Hui,Ji, Liangnian,Zhao, Cunyuan,&Mao, Zong-Wan.(2012).Mechanism of aquation and nucleobase binding of ruthenium (II) and osmium (II) arene complexes: A systematic comparison DFT study.JOURNAL OF ORGANOMETALLIC CHEMISTRY,704,17-28. |
MLA | Wang, Hanlu,et al."Mechanism of aquation and nucleobase binding of ruthenium (II) and osmium (II) arene complexes: A systematic comparison DFT study".JOURNAL OF ORGANOMETALLIC CHEMISTRY 704(2012):17-28. |
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