A Concerted Synchronous [2+2] Cycloreversion Repair Catalyzed by Two Electrons

被引：9

作者：

Davis, Daly ^{[1
]}

Bhushan, K. G. ^{[1
]}

Sajeev, Y. ^{[2
]}

Cederbaum, L. S. ^{[3
]}

机构：

[1] Bhabha Atom Res Ctr, Tech Phys Div, Bombay 400085, Maharashtra, India

[2] Bhabha Atom Res Ctr, Theoret Chem Sect, Bombay 400085, Maharashtra, India

[3] Heidelberg Univ, Phys Chem Inst, Theoret Chem, Neuenheimer Feld 229, D-69120 Heidelberg, Germany

来源：

JOURNAL OF PHYSICAL CHEMISTRY LETTERS | 2018年 / 9卷 / 24期

关键词：

PHOTOLYASE; MECHANISM; DIMERS;

D O I：

10.1021/acs.jpclett.8b03256

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The current understanding of photoenzyme-catalyzed [2 + 2] cycloreversion repair of cyclobutane pyrimidine dimer (CPD) is that a photogenerated electron from the photolyase enzyme catalyzes the repair. This one-electron catalyzed repair is a sequential two-bond breaking cycloreversion of the cyclobutane center and involves a negative ion radical as an intermediate. Here, by resonantly capturing two exogenous low-energy electrons into the molecular field of a CPD, we show that the concerted synchronous two-bond breaking reaction, which is intermediate-free, and hence a safe repair, is feasible through two-electron catalysis.

引用

页码：6973 / 6977

页数：9

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