含有Co4O4古巴活跃地点的人造金属蛋白
Lisa Olshansky1, Raúl Huerta-Lavorie2, Andy I Nguyen2
1Department of Chemistry, University of California, Irvine , Irvine, California 92697, United States.
Journal of the American Chemical Society
|February 6, 2018
概括
人工金属蛋白与基位模仿生物水氧化. 氨酸残留物中的键使得多电子的水氧化成为可能,将合成和自然系统连接起来.
科学领域:
- 生物有机化学 生物有机化学
- 催化剂是一种催化剂.
- 生物模拟化学 生物模拟化学
背景情况:
- 人工金属蛋白 (ArM) 是模仿自然金属酶功能的工程蛋白质.
- 四氧化物 (Co4O4) 库班核在结构上与光系统II和水氧化催化剂中的氧化复合物相似.
研究的目的:
- 为了构建人工金属蛋白与Co4O4古巴活体场所.
- 研究二次球相互作用,特别是键在调节水氧化反应中的作用.
- 为了弥合合成和生物水氧化系统之间的差距.
主要方法:
- 生物素-链维丁技术被用于固定蛋白质内的Co4O4古巴活性位点.
- 采用X射线晶体学来确定ARM的结构特征,包括键相互作用.
- 使用溶液电化学研究了ARM的氧化潜力和pH依赖反应性.
主要成果:
- 结晶学分析揭示了稳定的Co ((III) -OH2部分通过固定古巴位点的键.
- 有Ser和Phe残留的变体在pH8之前显示出主要的1e-/1H+化学物质,然后变得与pH无关.
- 在Co4O4位点附近引入Tyr残留物,形成单一的键,导致多e/多H+化学和pH值9.5的pH值依赖于pH值的机械转移,归因于Tyr脱.
结论:
- 二次球相互作用,特别是来自氨酸的键,对于人工金属蛋白中的多电子/多质子水氧化中介至关重要.
- 这些发现强调了蛋白质环境在控制金属酶的催化活性方面的重要性.
- 开发的ARM作为了解生物水氧化和合成水氧化催化剂的宝贵模型.
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