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通过有效的QM/MM方法探索Renilla中的发光剂

Ashim Nandi¹, Aoxuan Zhang¹, Zhen Tao Chu¹

¹Department of Chemistry, University of Southern California, Los Angeles, California 90089-1062, United States.

Journal of the American Chemical Society

|May 8, 2024

概括

生物发光涉及生物体的光产生. 这项研究揭示了coelenteramide的酸盐状态是Renilla luciferase 8 (RLuc8) 发光的关键,而质子转移影响了这一过程.

科学领域:

生物化学
生物物理
计算化学

背景情况:

生物发光是生物通过生物化学反应发出的光.
来自Renilla reniformis的光酶 (RLuc) 发出蓝光,并用于生物发光标记.
RLuc8是一种RLuc的变体,具有八种氨基酸替代.

研究的目的:

研究RLuc8中的发光物种和质子转移 (PT) 机制.
了解蛋白质结构在调节生物发光中的作用.
验证用于研究光蛋白中的染色体状态和PT的计算方法.

主要方法:

量子力学一致力场 (QM/MM-FD) 方法.
半宏观蛋白质双极-朗格温双极 (PDLD/S) 方法与线性响应近似.
对RLuc8及其变体 (RLuc8-D120A,RLuc8-D162A,AncFT-D160A) 的计算建模.

主要成果:

在RLuc8中,coelenteramide的酸盐状态被确定为主要发光物种.
从中性胆胺转移到Asp162对于生物发光至关重要.
计算模型准确地复制了各种RLuc8变体和AncFT-D160A的实验性排放最大值.

结论:

该研究证实了coelenteramide作为RLuc8中的发射剂的酸盐状态.
质子转移机制显著影响生物发光光谱.
计算方法为研究光蛋白中的PT和设计新生物发光系统提供了强大的框架.

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