Dynamics and mechanisms of DNA repair by photolyase.
Dynamics and mechanisms of DNA repair by photolyase.
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DOI：
10.1039/c4cp05286b
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发表时间：
2015-05-14
期刊：
影响因子：
--
通讯作者：
Zhong D
中科院分区：
文献类型：
--
作者：
Liu Z;Wang L;Zhong D
光裂解酶是一类黄素蛋白，使用蓝光修复两种类型的紫外线诱导的 DNA 损伤：环丁烷嘧啶二聚体 (CPD) 和嘧啶-嘧啶酮 (6–4) 光产物 (6–4PP)。从这个角度来看，我们回顾了光裂合酶修复两种类型 DNA 修复动力学和机制的最新进展。我们首先报道了黄素在各种氧化还原态下的光谱表征以及光裂合酶中活性位点溶剂化动力学。然后，我们通过解决超快时间尺度上的所有基本步骤，包括多个分子间电子和质子转移反应以及键断裂和形成过程，系统地总结了光裂合酶和仿生系统对受损 DNA 的详细修复动力学。我们确定了独特的电子隧道通路，识别了关键的功能残基，揭示了高修复效率的分子起源，从而从最根本的层面阐明了分子机制和修复光循环。我们最终得出的结论是，与仿生系统的水溶液不同，光裂合酶的活性位点提供了独特的静电环境和局部灵活性，从而为所有基本动力学提供了专用的协同作用，以最大限度地提高修复效率。这种修复光机是第一个将整个功能进化完全实时绘制出来的酶。
Photolyase, a class of flavoproteins, uses blue light to repair two types of ultraviolet-induced DNA damage, cyclobutane pyrimidine dimer (CPD) and pyrimidine-pyrimidone (6–4) photoproduct (6–4PP). In this perspective, we review the recent progress on the repair dynamics and mechanisms of both types of DNA restoration by photolyases. We first report the spectroscopic characterization of flavin in various redox states and the active-site solvation dynamics in photolyases. We then systematically summarize the detailed repair dynamics of damaged DNA by photolyases and a biomimetic system through resolving all elementary steps on the ultrafast timescales, including multiple intermolecular electron- and proton-transfer reactions and bond-breaking and -making processes. We determined the unique electron tunneling pathways, identified the key functional residues and revealed the molecular origin of high repair efficiency, and thus elucidate the molecular mechanisms and repair photocycles at the most fundamental level. We finally conclude that the active sites of photolyases, unlike aqueous solution for the biomimetic system, provide a unique electrostatic environment and local flexibility and thus a dedicated synergy for all elementary dynamics to maximize the repair efficiency. This repair photomachine is the first enzyme that the entire functional evolution is completely mapped out in real time.
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影响因子：
3.2
作者：
Boussicault, F;Kr端ger, O;Wille, U
通讯作者：
Wille, U
影响因子：
15
作者：
Chang, Chih-Wei;He, Ting-Fang;Guo, Lijun;Stevens, Jeffrey A.;Li, Tanping;Wang, Lijuan;Zhong, Dongping
通讯作者：
Zhong, Dongping
影响因子：
--
作者：
COPELAND, RA;SPIRO, TG
通讯作者：
SPIRO, TG
色氨酸7-卤代酶（PRNA）结构提出了一种区域选择性氯化的机制。
DOI：
10.1126/science.1116510
发表时间：
2005-09-30
期刊：
Science (New York, N.Y.)
影响因子：
--
作者：
Dong C;Flecks S;Unversucht S;Haupt C;van Pée KH;Naismith JH
通讯作者：
Naismith JH
影响因子：
2.9
作者：
GHISLA, S;MASSEY, V;MAYHEW, SG
通讯作者：
MAYHEW, SG