Department of Biochemistry and Microbiology, Faculty of Science, Agriculture and Engineering, University of Zululand, KwaDlangezwa 3886, South Africa.
Faculty of Medicine, Health and Life Sciences, Swansea University, Swansea SA2 8PP, UK.
Biomolecules. 2023 Dec 1;13(12):1733. doi: 10.3390/biom13121733.
Cytochrome P450 monooxygenases (CYPs; P450s) are a superfamily of heme-containing enzymes that are recognized for their vast substrate range and oxidative multifunctionality. CYP107 family members perform hydroxylation and epoxidation processes, producing a variety of biotechnologically useful secondary metabolites. Despite their biotechnological importance, a thorough examination of CYP107 protein structures regarding active site cavity dynamics and key amino acids interacting with bound ligands has yet to be undertaken. To address this research knowledge gap, 44 CYP107 crystal structures were investigated in this study. We demonstrate that the CYP107 active site cavity is very flexible, with ligand binding reducing the volume of the active site in some situations and increasing volume size in other instances. Polar interactions between the substrate and active site residues result in crucial salt bridges and the formation of proton shuttling pathways. Hydrophobic interactions, however, anchor the substrate within the active site. The amino acid residues within the binding pocket influence substrate orientation and anchoring, determining the position of the hydroxylation site and hence direct CYP107's catalytic activity. Additionally, the amino acid dynamics within and around the binding pocket determine CYP107's multifunctionality. This study serves as a reference for understanding the structure-function analysis of CYP107 family members precisely and the structure-function analysis of P450 enzymes in general. Finally, this work will aid in the genetic engineering of CYP107 enzymes to produce novel molecules of biotechnological interest.
细胞色素 P450 单加氧酶(CYPs;P450s)是一类血红素酶超家族,以其广泛的底物范围和氧化多功能性而闻名。CYP107 家族成员执行羟化和环氧化过程,产生各种具有生物技术用途的次级代谢物。尽管它们具有生物技术的重要性,但对于 CYP107 蛋白结构的活性位点腔动力学和与结合配体相互作用的关键氨基酸的全面研究尚未进行。为了解决这一研究知识差距,本研究调查了 44 种 CYP107 晶体结构。我们证明 CYP107 的活性位点腔非常灵活,在某些情况下,配体结合会降低活性位点的体积,而在其他情况下则会增加体积大小。底物与活性位点残基之间的极性相互作用导致关键的盐桥形成和质子穿梭途径的形成。然而,疏水性相互作用将底物锚定在活性位点内。结合口袋内的氨基酸残基影响底物的取向和锚定,决定羟化位点的位置,从而直接影响 CYP107 的催化活性。此外,结合口袋内和周围的氨基酸动力学决定了 CYP107 的多功能性。本研究为精确理解 CYP107 家族成员的结构-功能分析以及 P450 酶的结构-功能分析提供了参考。最后,这项工作将有助于对 CYP107 酶进行基因工程改造,以生产具有生物技术兴趣的新型分子。