光活性黄色蛋白中的低屏障键:在晶体和溶液中缺少的真空工件
Timo Graen1, Ludger Inhester2, Maike Clemens1
1Max Planck Institute for Biophysical Chemistry , Am Faßberg 11, 37077 Göttingen, Germany.
Journal of the American Chemical Society
|December 15, 2016
概括
这项研究质疑光活性黄色蛋白 (PYP) 中存在低屏障键 (LBHB),提出了一个更适合无核量子效应的实验数据的替代模型.
科学领域:
- 生物物理
- 结构生物学
- 计算化学
背景情况:
- 在光活性黄色蛋白 (PYP) 中存在低屏障键 (LBHB) 是有争议的.
- 之前的研究表明中性Arg52残留会触发LBHB的形成.
研究的目的:
- 提供与现有数据一致的LBHB形成的替代模型.
- 调查晶体环境和Arg52质子化状态对LBHB的作用.
主要方法:
- 分析中子衍射结构因子.
- 在晶体,溶液和真空条件下的分子动力学 (MD) 模拟.
- 三维核平衡密度计算
主要成果:
- 提出了一种替代模型,解释了无核量子效应的质子Arg52的键长度增加.
- 模拟显示晶体环境稳定了Arg52的键,并预测了pKa的上升.
- 真空计算引入了有利于LBHB和大型1H NMR化学转移的工件.
结论:
- 晶体环境, 而不是真空条件, 准确地描述了PYP.
- 提出的模型解释了实验数据,并提出了以前的解释中的异常.
- 在没有特定环境因素的生理条件下,PYP中的LBHB不太可能发生.
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