Department of Chemistry, University of Southern California, Los Angeles, California 90089-1062, United States.
J Am Chem Soc. 2022 Jan 26;144(3):1251-1257. doi: 10.1021/jacs.1c10494. Epub 2022 Jan 13.
The cleavage of protein inside cell membranes regulates pathological pathways and is a subject of major interest. Thus, the nature of the coupling between the physical environment and the function of such proteins has recently attracted significant experimental and theoretical efforts. However, it is difficult to determine the nature of this coupling uniquely by experimental and theoretical studies unless one can separate the chemical and the environmental factors. This work describes calculations of the activation barriers of the intramembrane rhomboid protease in neutral and charged lipid bilayers and in detergent micelle, trying to explore the environmental effect. The calculations of the chemical barrier are done using the empirical valence bond (EVB) method. Additionally, the renormalization method captures the energetics and dynamical effects of the conformational change. The simulations indicate that the physical environment around the rhomboid protease is not a major factor in changing the chemical catalysis and that the conformational and substrate dynamics do not exhibit long-time coupling. General issues about the action of membrane-embedded enzymes are also considered.
细胞膜内蛋白质的裂解调节着病理途径,是一个主要的研究课题。因此,物理环境与这类蛋白质功能之间的偶联本质最近引起了大量的实验和理论研究。然而,除非能够分离化学和环境因素,否则仅通过实验和理论研究很难确定这种偶联的本质。本工作描述了在中性和带电脂质双层以及去污剂胶束中,内膜菱形蛋白酶的激活势垒的计算,试图探索环境效应。化学势垒的计算使用经验价键(EVB)方法进行。此外,重整化方法捕捉构象变化的能量和动力学效应。模拟表明,菱形蛋白酶周围的物理环境不是改变化学催化的主要因素,构象和底物动力学没有表现出长时间的耦合。还考虑了关于膜嵌入酶作用的一般问题。