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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
Source PublicationJOURNAL OF ORGANOMETALLIC CHEMISTRY
Volume704Pages:17-28
Abstract

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.

SubtypeArticle
KeywordDft Ruthenium Osmium Aquation Nucleobase Pk(a)
WOS HeadingsScience & Technology ; Physical Sciences
DOI10.1016/j.jorganchem.2011.12.034
WOS Subject ExtendedChemistry
WOS KeywordEFFECTIVE CORE POTENTIALS ; CANCER-CELL CYTOTOXICITY ; ANTICANCER COMPLEXES ; ORGANOMETALLIC RUTHENIUM(II) ; MOLECULAR CALCULATIONS ; DNA-BINDING ; ANTITUMOR COMPLEXES ; CISPLATIN BINDING ; SOLVATION METHODS ; OVARIAN-CANCER
Indexed BySCI
Language英语
WOS SubjectChemistry, Inorganic & Nuclear ; Chemistry, Organic
WOS IDWOS:000300638400003
Citation statistics
Cited Times:6[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.giec.ac.cn/handle/344007/10181
Collection中国科学院广州能源研究所
Affiliation1.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
Recommended Citation
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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