A Concerted Synchronous [2 + 2] Cycloreversion Repair Catalyzed by Two Electrons,The Journal of Physical Chemistry Letters

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A Concerted Synchronous [2 + 2] Cycloreversion Repair Catalyzed by Two Electrons
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2018-11-27 00:00:00 , DOI: 10.1021/acs.jpclett.8b03256
Daly Davis , K. G. Bhushan , Y. Sajeev , L. S. Cederbaum ₁

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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.

中文翻译：

两电子催化的同步同步[2 + 2]循环返修

对光酶催化的环丁烷嘧啶二聚体（CPD）的[2 + 2]环还原修复的当前理解是，来自光解酶的光生电子催化修复。该单电子催化的修复是环丁烷中心的连续的两键断裂环还原，并且涉及负离子自由基作为中间体。在这里，通过共振将两个外源低能电子捕获到CPD的分子场中，我们表明通过双电子催化，协同的同步双键断裂反应是无中间体的，因此安全修复，是可行的。

更新日期：2018-11-27

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