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首页> 外文期刊>Proceedings of the National Academy of Sciences of the United States of America >Alternative ground states enable pathway switching in biological electron transfer
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Alternative ground states enable pathway switching in biological electron transfer

机译：替代基态可实现生物电子转移中的路径切换

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摘要

Electron transfer is the simplest chemical reaction and constitutes the basis of a large variety of biological processes, such as photosynthesis and cellular respiration. Nature has evolved specific proteins and cofactors for these functions. The mechanisms optimizing biological electron transfer have been matter of intense debate, such as the role of the protein milieu between donor and acceptor sites. Here we propose a mechanism regulating long-range electron transfer in proteins. Specifically, we report a spec-troscopic, electrochemical, and theoretical study on WT and single-mutant Cu_A redox centers from Thermus thermophilus, which shows that thermal fluctuations may populate two alternative ground-state electronic wave functions optimized for electron entry and exit, respectively, through two different and nearly perpendicular pathways. These findings suggest a unique role for alternative or "invisible" electronic ground states in directional electron transfer. Moreover, it is shown that this energy gap and, therefore, the equilibrium between ground states can be fine-tuned by minor perturbations, suggesting alternative ways through which protein-protein interactions and membrane potential may optimize and regulate electron-proton energy transduction.
机译：电子转移是最简单的化学反应，并构成许多生物过程（例如光合作用和细胞呼吸）的基础。大自然已经进化出特定的蛋白质和辅助因子来实现这些功能。优化生物电子转移的机制一直是争论不休的问题，例如供体和受体位点之间蛋白质环境的作用。在这里，我们提出了一种调节蛋白质中远距离电子转移的机制。具体来说，我们报告了对嗜热栖热菌的WT和单突变Cu_A氧化还原中心的光谱，电化学和理论研究，结果表明，热涨落可能会分别填充为电子的进入和退出而优化的两个可选基态电子波函数。 ，通过两种不同且几乎垂直的途径。这些发现表明在定向电子转移中，替代性或“不可见”电子基态的独特作用。此外，表明该能隙以及因此基态之间的平衡可以通过较小的扰动来微调，这表明蛋白质-蛋白质相互作用和膜电位可以优化和调节电子-质子能量传导的替代方法。

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  • 作者

    Luciano A. Abriata; Damian alvarez-Paggi; Gabriela N. Ledesma; Ninian J. Blackburn; alejandro J. Vila; Daniel H. Murgida;

  • 作者单位

    Instituto de Biologia Molecular y Celular de Rosario, Consejo Nacional de Investigaciones Cientificas y Tecnicas, Facultad de Ciencias Bioquimicas y Farmaceuticas, Universidad Nacional de Rosario, S2002LRK Rosario, Argentina;

    Departamento de Quimica Inorganica, Analitica y Quimica Fisica and Instituto de Quimica Fisica de los Materiales, Medio Ambiente y Energia (INQUIMAE), Consejo Nacional de Investigaciones Cientificas y Tecnicas, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos Aires, C1428EHA Buenos Aires, Argentina;

    Instituto de Quimica Rosario, Consejo Nacional de Investigaciones Cientificas y Tecnicas, Facultad de Ciencias Bioquimicas y Farmaceuticas, Universidad Nacional de Rosario, S2002LRK Rosario, Argentina;

    Institute of Environmental'Health, Oregon Health and Sciences University, Beaverton, OR 97006;

    Instituto de Biologia Molecular y Celular de Rosario, Consejo Nacional de Investigaciones Cientificas y Tecnicas, Facultad de Ciencias Bioquimicas y Farmaceuticas, Universidad Nacional de Rosario, S2002LRK Rosario, Argentina;

    Departamento de Quimica Inorganica, Analitica y Quimica Fisica and Instituto de Quimica Fisica de los Materiales, Medio Ambiente y Energia (INQUIMAE), Consejo Nacional de Investigaciones Cientificas y Tecnicas, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos Aires, C1428EHA Buenos Aires, Argentina;

  • 收录信息 美国《科学引文索引》(SCI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    cytochrome oxidase; invisible states; paramagnetic proteins; NMR; spectroscopy;

    机译：细胞色素氧化酶隐形状态顺磁性蛋白NMR;光谱学;

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