光系II中的氧气进化的Mn团:高分辨率晶体结构中的质子化模式和氧化状态
Artur Galstyan1, Arturo Robertazzi, Ernst Walter Knapp
1Department of Biology, Chemistry and Pharmacy, Institute of Chemistry and Biochemistry, Freie Universität Berlin, Fabeckstrasse 36a, D-14195 Berlin, Germany.
Journal of the American Chemical Society
|April 12, 2012
概括
量子化学计算显示,光系II中的氧气演变的Mn星团并非处于S(1) 状态. 结构是减少状态的混合物,主要是S(-3) 状态 (Mn(II,II,III,III)).
科学领域:
- 生物化学 生物化学
- 量子化学 是一个量子化学.
- 光合作用研究研究 光合作用研究
背景情况:
- 光系统II (PSII) 对于氧光合作用至关重要.
- 在PSII内的氧气进化的Mn集群促进了水的氧化.
- 确定Mn团的质子化和氧化状态是理解PSII功能的关键.
研究的目的:
- 确定PSII的高分辨率晶体结构中的Mn团的质子化模式和氧化状态.
- 为了研究实验结构的S状态.
- 识别潜在的替代质子状态及其相关性.
主要方法:
- 广泛的量子化学密度功能理论 (DFT) 计算.
- 对光系统II的高分辨率 (1.9 Å) 晶体结构的分析.
主要成果:
- 实验中的晶体结构不太可能代表S(1) 状态.
- 确定并讨论了有限数量的替代质子化模式.
- 结构是状态的混合物,其中显著贡献 (~60%) 来自S(-3) 状态,其特征是Mn(II,II,III,III) 氧化状态.
结论:
- 通常描绘的S(1) 状态可能不会准确地反映研究的晶体结构.
- 团存在于减少氧化状态的混合物中,挑战了以前的假设.
- 这些发现为光系统II中的水氧化机制提供了新的见解.
相关概念视频
Photosystem II
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Oxygenic Photosynthesis
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