Theoretical studies on DNA-photocleavage efficiencies of Ru(II) polypyridyl complexes

被引：11

作者：

Miao, Ti-Fang ^{[1
]}

Li, Shuang ^{[1
]}

Chen, Jin-Can ^{[2
]}

Wang, Na-Li ^{[1
]}

Zheng, Kang-Cheng ^{[3
]}

机构：

[1] Huaibei Normal Univ, Coll Chem & Mat Sci, Huaibei 235000, Peoples R China

[2] Guangdong Med Coll, Anal Ctr, Zhanjiang 524023, Peoples R China

[3] Sun Yat Sen Univ, Sch Chem & Chem Engn, Key Lab Bioinorgan & Synthet Chem, Minist Educ, Guangzhou 510275, Guangdong, Peoples R China

来源：

DALTON TRANSACTIONS | 2013年 / 42卷 / 07期

基金：

中国国家自然科学基金;

关键词：

ELECTRON-TRANSFER REACTIONS; EFFECTIVE CORE POTENTIALS; MOLECULAR CALCULATIONS; CHIRAL COMPLEXES; EXCITED-STATES; OXIDATION; RUTHENIUM; ENERGIES; PROTEINS; GUANINE;

D O I：

10.1039/c2dt31998e

中图分类号：

O61 [无机化学];

学科分类号：

070301 ; 081704 ;

摘要：

Theoretical studies on the DNA-photocleavage efficiencies of Ru(II) polypyridyl complexes 1-4 have been carried out using density functional theory (DFT). First, an evaluation of the computational accuracy of the redox potentials for [Ru(bpy)(3)](2+) in the ground state and the excited state was tested by different computational methods. Secondly, the redox potentials of complexes 1-4 in the excited state were accurately computed. Finally, the trend in the DNA-photocleavage efficiencies (phi) of complexes 1-4, i.e., phi(4) > phi(3) > phi(2) > phi(1), were reasonably explained by the excited-state reduction potentials and the electron-transfer activation energies. In particular, the DNA-photocleavage efficiencies of two new Ru(II) complexes 3 and 4 were predicted.

引用

页码：2463 / 2468

页数：6

共 34 条

[1] Quantum calculation of molecular energies and energy gradients in solution by a conductor solvent model [J].

Barone, V ;

Cossi, M .

JOURNAL OF PHYSICAL CHEMISTRY A, 1998, 102 (11) :1995-2001

[2] Photoinduced intramolecular electron transfer in ruthenium and osmium polyads:: Insights from theory [J].

Ciofini, I ;

Lainé, PP ;

Bedioui, F ;

Adamo, C .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2004, 126 (34) :10763-10777

[3] Energies, structures, and electronic properties of molecules in solution with the C-PCM solvation model [J].

Cossi, M ;

Rega, N ;

Scalmani, G ;

Barone, V .

JOURNAL OF COMPUTATIONAL CHEMISTRY, 2003, 24 (06) :669-681

[4] Characterization of the relevant excited states in the photodissociation of CO-ligated hemoglobin and myoglobin [J].

Dreuw, A ;

Dunietz, BD ;

Head-Gordon, M .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2002, 124 (41) :12070-12071

[5] Biomedical uses and applications of inorganic chemistry. An overview [J].

Farrell, N .

COORDINATION CHEMISTRY REVIEWS, 2002, 232 (1-2) :1-4

[6] TOWARD A SYSTEMATIC MOLECULAR-ORBITAL THEORY FOR EXCITED-STATES [J].

FORESMAN, JB ;

HEADGORDON, M ;

POPLE, JA ;

FRISCH, MJ .

JOURNAL OF PHYSICAL CHEMISTRY, 1992, 96 (01) :135-149

[7]

Frisch M. J., 2010, GAUSSIAN 09

[8]

Frisch M.J., 2004, Gaussian 09

[9]

HAY PJ, 1985, J CHEM PHYS, V82, P299, DOI [10.1063/1.448800, 10.1063/1.448799]

[10] Probing the mechanism of hypoxia selectivity of copper bis(thiosemicarbazonato) complexes: DFT calculation of redox potentials and absolute acidities in solution [J].

Holland, JP ;

Green, JC ;

Dilworth, JR .

DALTON TRANSACTIONS, 2006, (06) :783-794

← 1 2 3 4 →