Mechanistic Insights Into the Factors That Influence the DNA Nuclease Activity of Mononuclear Facial Copper Complexes Containing Hetero-Substituted Cyclens
Mechanistic Insights Into the Factors That Influence the DNA Nuclease Activity of Mononuclear Facial Copper Complexes Containing Hetero-Substituted Cyclens
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影响含异取代 Cyclens 的单核面部铜复合物 DNA 核酸酶活性因素的机制见解
DOI：
10.1021/acscatal.5b01735
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发表时间：
2016-01
期刊：
影响因子：
12.9
通讯作者：
Zhao Cunyuan
中科院分区：
文献类型：
--
作者：
Zhang Xuepeng;Liu Xueping;Phillips David Lee;Zhao Cunyuan
采用密度泛函理论（DFT）方法系统研究了含杂取代大环内酯的单核铜配合物的DNA核酸酶活性的影响因素。cyclen的杂取代被发现显着影响的单核Cu（II）配合物的二聚化趋势检查和各自的金属键合的水分子的pKa值。研究发现，铜（II）-氧杂环烯配合物更有利于DNA二核苷酸类似物BNPP-（双（对硝基苯基）磷酸）的水解切割。这是由于该物种具有较高的二聚化抗性以产生较高浓度的活性催化剂和较低的Cu（II）配位的水分子的pKa值以促进更容易产生更好的亲核羟基离子，这给出了较低的反应势垒。测定了配合物的二聚化反应和相应的氧化还原电位，并对配合物的二聚化反应进行了讨论。
The factors that influence the DNA nuclease activity of mononuclear facial copper complexes containing heterosubstituted cyclens were systematically investigated in this work using density functional theory (DFT) calculations. The heterosubstitution of cyclens were found to significantly affect the dimerization tendency of the mononuclear Cu(II) complexes examined and their respective pKa values of the metal-bonded water molecules. The Cu(II)–oxacyclen complex was found to be more favorable for the hydrolytic cleavage of the DNA dinucleotide analogue BNPP–(bis (p-nitrophenyl) phosphate). This was due to this species having a higher dimerization resistance to give rise to a higher concentration of the active catalyst and a lower pKa value of the Cu(II)-coordinated water molecule to facilitate an easier generation of the better nucleophile hydroxyl ion, which gave a lower reaction barrier. The dimerization of the Cu(I) complexes studied and their corresponding redox potentials were determined, and a remarka...
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DOI：
10.1002/cber.19610940602
发表时间：
1961-06
期刊：
Chemische Berichte
影响因子：
--
作者：
H. Stetter;K. Mayer
通讯作者：
H. Stetter;K. Mayer
影响因子：
4.4
作者：
HAY, PJ;WADT, WR
通讯作者：
WADT, WR
影响因子：
15
作者：
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通讯作者：
R. Sarangi;S. I. Gorelsky;L. Basumallick;H. Hwang;R. Pratt;T. Stack;Yi Lu;K. Hodgson;B. Hedman;E. Solomon
DOI：
10.1021/jp811388w
发表时间：
2009-05
期刊：
The journal of physical chemistry. A
影响因子：
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作者：
L. Roy;E. Jakubikova;M. Guthrie;E. Batista
通讯作者：
L. Roy;E. Jakubikova;M. Guthrie;E. Batista
DOI：
10.1002/chin.200644271
发表时间：
2006-10
期刊：
ChemInform
影响因子：
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作者：
W. Cleland;A. Hengge
通讯作者：
W. Cleland;A. Hengge