School of Pharmacy, University of Connecticut, Storrs, CT 06269, USA.
Department of Pharmaceutical Sciences, Albany College of Pharmacy and Health Sciences, 106 New Scotland Avenue, Albany, NY 12208, USA.
Int J Mol Sci. 2018 Mar 29;19(4):1025. doi: 10.3390/ijms19041025.
The over two dozen CYP2B structures of human, rabbit, and woodrat enzymes solved in the last decade have significantly enhanced our understanding of the structure-function relationships of drug metabolizing enzymes. More recently, an important role has emerged for halogen-π interactions in the CYP2B6 active site in substrate selectivity, explaining in part the preference for halogenated ligands as substrates. The mechanism by which such ligands interact with CYP2B enzymes involves conserved phenylalanine side chains, in particular F108, F115, or F297, in the active site, which form π bonds with halogens. To illustrate such halogen-π interactions using drugs that are major substrates of CYP2B6, we present here a crystal structure of CYP2B6 in complex with an analog of the widely used anti-HIV drug efavirenz, which contains a methyl group in place of the carbonyl oxygen. The chlorine of the efavirenz analog forms a π bond with the aromatic ring of F108, whereas the putative metabolism site on the distal end of the molecule is oriented towards the heme iron. The crystal structure showcases how CYP2B6 accommodates this important drug analog of considerable size in the active site by movement of various side chains without substantially increasing the active site volume. Furthermore, the CYP2B6-efavirenz analog complex provides a useful platform to investigate computationally as well as biophysically the effect of genetic polymorphisms on binding of the widely studied efavirenz.
过去十年中,人类、兔和林鼠的二十多种 CYP2B 结构已被成功解析,这极大地促进了我们对药物代谢酶结构与功能关系的理解。最近,卤原子-π 相互作用在 CYP2B6 活性部位对底物选择性中发挥了重要作用,部分解释了卤代配体作为底物的偏好性。这种配体与 CYP2B 酶相互作用的机制涉及活性部位保守的苯丙氨酸侧链,特别是 F108、F115 或 F297,它们与卤素形成π键。为了用 CYP2B6 的主要底物药物来说明这种卤原子-π 相互作用,我们在此展示了 CYP2B6 与广泛使用的抗 HIV 药物依非韦伦类似物的复合物的晶体结构,其中含有一个甲基取代了羰基氧。依非韦伦类似物的氯与 F108 的芳环形成π键,而分子远端的假定代谢部位则朝向血红素铁。晶体结构展示了 CYP2B6 如何通过各种侧链的移动来适应这个在活性部位具有相当大尺寸的重要药物类似物,而不会显著增加活性部位的体积。此外,CYP2B6-依非韦伦类似物复合物为广泛研究的依非韦伦的结合遗传多态性的计算和生物物理研究提供了一个有用的平台。