科克的光合作用水氧化时钟中间体的结构
Jan Kern1, Ruchira Chatterjee1, Iris D Young1
1Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA.
Nature
|November 9, 2018
概括
研究人员使用X射线晶体学可视化了光合作用氧气进化周期的所有状态. 他们揭示了结构变化,并确定了参与氧气生产的关键水分子,排除了O-O键形成的某些机制.
科学领域:
- 生物化学 生物化学
- 光合作用研究研究光合作用.
- 结构生物学是结构生物学.
背景情况:
- 光合作用氧的进化,对生命至关重要,遵循Kok的S状态周期.
- 光系II (PSII) 中的氧进化复合体 (OEC) 包含一个负责氧化水的Mn4CaO5集群.
- 了解O-O键形成的精确机制仍然是光合作用研究中的一个关键挑战.
研究的目的:
- 在PSII中以高分辨率可视化Kok的S状态周期的所有 (元) 稳定状态.
- 为了捕捉催化循环期间的短暂结构变化.
- 阐明在水氧化过程中O-O键形成和基质输送的机制.
主要方法:
- 在室温下进行连续的秒X射线晶体学 (SFX).
- 同时的X射线发射光谱 (XES) 与多闪光可见激光激发.
- 对OEC的 (元) 稳定和过渡状态的高分辨率结构确定.
主要成果:
- 获得了所有 (元) 稳定的S0-S3状态的高分辨率结构 (2.042.08 Å).
- 在150和400微秒的两个过渡状态的结构显示出显著的结构动态.
- 在S2→S3过渡期间观察到额外的氧原子 (Ox) 结合,位于Ca和Mn1之间.
- 鉴定出水联体W3可能参与基质输送.
结论:
- 在S3状态下Ox的结合支持O5是基质,Ox是第二基质或在O2释放后重新填补O5位置的机制.
- 在S3状态中排除过氧键的形成.
- 涉及W3和W2的核友攻击机制不太可能形成O-O键.
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