激活一个开放的外,碳酸桥梁的二铁复合体,以结合二
Charles H Arnett1, Theodor Agapie1
1Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, California 91125, United States.
Journal of the American Chemical Society
|April 15, 2020
概括
研究人员模拟了酶
科学领域:
- 生物有机化学
- 有机金属化学
- 催化剂
背景情况:
- 对于N2结合的基酶FeMo辅助因子激活的理解很少.
- 结晶学表明N2减少发生在碳桥接二位点.
研究的目的:
- 模拟N2结合的Fe-(μ-C) -Fe位点的激活.
- 合成和表征一种新的双核六素配体及其二铁μ-卡宾复合物.
主要方法:
- 六素连接体及其二铁μ-卡宾复合物的合成.
- 使用SQUID磁力测量,Mössbauer光谱和DFT计算进行表征.
- 涉及H+,e和N2结合的机制研究.
主要成果:
- 合成了具有S=1基态的独特的二铁μ-碳化合物 (P6ArC) Fe2{\displaystyle {P6ArC}Fe2}{\displaystyle {P6Fe}Fe2}{\displaystyle {P6ArC}Fe2}{\displaystyle {P6Fe}Fe1}H}).
- 在添加H+/e-源时,该复合物被激活到N2结合.
- 已确定一种能够协调N2的铁碳酸中间体.
结论:
- 这项研究提供了酶中FeMo辅因子的还原激活模型.
- 一个新的Fe (μ-carbyne) (μ-H) Fe基因被描述.
- 获得了关于铁中心N2结合和减少机制的见解.
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