GIEC OpenIR  > 中国科学院广州能源研究所
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
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
DOI10.1016/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.
条目包含的文件
文件名称/大小 文献类型 版本类型 开放类型 使用许可
Mechanism of aquatio(1802KB)期刊论文作者接受稿限制开放CC BY-NC-SA请求全文
个性服务
推荐该条目
保存到收藏夹
查看访问统计
导出为Endnote文件
谷歌学术
谷歌学术中相似的文章
[Wang, Hanlu]的文章
[DeYonker, Nathan J.]的文章
[Gao, Hui]的文章
百度学术
百度学术中相似的文章
[Wang, Hanlu]的文章
[DeYonker, Nathan J.]的文章
[Gao, Hui]的文章
必应学术
必应学术中相似的文章
[Wang, Hanlu]的文章
[DeYonker, Nathan J.]的文章
[Gao, Hui]的文章
相关权益政策
暂无数据
收藏/分享
所有评论 (0)
暂无评论
 

除非特别说明,本系统中所有内容都受版权保护,并保留所有权利。