基于黄素的电子分叉实现能量守恒的机制洞察。
Mechanistic insights into energy conservation by flavin-based electron bifurcation.
作者信息
Lubner Carolyn E, Jennings David P, Mulder David W, Schut Gerrit J, Zadvornyy Oleg A, Hoben John P, Tokmina-Lukaszewska Monika, Berry Luke, Nguyen Diep M, Lipscomb Gina L, Bothner Brian, Jones Anne K, Miller Anne-Frances, King Paul W, Adams Michael W W, Peters John W
机构信息
Biosciences Center, National Renewable Energy Laboratory, Golden, Colorado, USA.
School of Molecular Sciences, Arizona State University, Tempe, Arizona, USA.
出版信息
Nat Chem Biol. 2017 Jun;13(6):655-659. doi: 10.1038/nchembio.2348. Epub 2017 Apr 10.
Abstract
The recently realized biochemical phenomenon of energy conservation through electron bifurcation provides biology with an elegant means to maximize utilization of metabolic energy. The mechanism of coordinated coupling of exergonic and endergonic oxidation-reduction reactions by a single enzyme complex has been elucidated through optical and paramagnetic spectroscopic studies revealing unprecedented features. Pairs of electrons are bifurcated over more than 1 volt of electrochemical potential by generating a low-potential, highly energetic, unstable flavin semiquinone and directing electron flow to an iron-sulfur cluster with a highly negative potential to overcome the barrier of the endergonic half reaction. The unprecedented range of thermodynamic driving force that is generated by flavin-based electron bifurcation accounts for unique chemical reactions that are catalyzed by these enzymes.
摘要
最近通过电子分叉实现的能量守恒生化现象为生物学提供了一种优化代谢能量利用的巧妙方法。通过光学和顺磁光谱研究阐明了单一酶复合物对放能和吸能氧化还原反应进行协调偶联的机制，揭示了前所未有的特征。通过生成低电位、高能、不稳定的黄素半醌并将电子流导向具有高度负电位的铁硫簇以克服吸能半反应的障碍，电子对在超过1伏特的电化学势上发生分叉。基于黄素的电子分叉产生的前所未有的热力学驱动力范围解释了这些酶催化的独特化学反应。
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