Shaw Daniel J, Waters Lorna C, Strong Sarah L, Schulze Monika-Sarah E D, Greetham Gregory M, Towrie Mike, Parker Anthony W, Prosser Christine E, Henry Alistair J, Lawson Alastair D G, Carr Mark D, Taylor Richard J, Hunt Neil T, Muskett Frederick W
Department of Chemistry and York Biomedical Research Institute, University of York Heslington York YO19 5DD UK
Department of Molecular and Cell Biology/Leicester Institute of Structural and Chemical Biology, University of Leicester, University Road Leicester LE1 7RH UK
Chem Sci. 2023 Jun 16;14(27):7524-7536. doi: 10.1039/d3sc00728f. eCollection 2023 Jul 12.
Knowledge of protein dynamics is fundamental to the understanding of biological processes, with NMR and 2D-IR spectroscopy being two of the principal methods for studying protein dynamics. Here, we combine these two methods to gain a new understanding of the complex mechanism of a cytokine:receptor interaction. The dynamic nature of many cytokines is now being recognised as a key property in the signalling mechanism. Interleukin-17s (IL-17) are proinflammatory cytokines which, if unregulated, are associated with serious autoimmune diseases such as psoriasis, and although there are several therapeutics on the market for these conditions, small molecule therapeutics remain elusive. Previous studies, exploiting crystallographic methods alone, have been unable to explain the dramatic differences in affinity observed between IL-17 dimers and their receptors, suggesting there are factors that cannot be fully explained by the analysis of static structures alone. Here, we show that the IL-17 family of cytokines have varying degrees of flexibility which directly correlates to their receptor affinities. Small molecule inhibitors of the cytokine:receptor interaction are usually thought to function by either causing steric clashes or structural changes. However, our results, supported by other biophysical methods, provide evidence for an alternate mechanism of inhibition, in which the small molecule rigidifies the protein, causing a reduction in receptor affinity. The results presented here indicate an induced fit model of cytokine:receptor binding, with the more flexible cytokines having a higher affinity. Our approach could be applied to other systems where the inhibition of a protein-protein interaction has proved intractable, for example due to the flat, featureless nature of the interface. Targeting allosteric sites which modulate protein dynamics, opens up new avenues for novel therapeutic development.
蛋白质动力学知识对于理解生物过程至关重要,核磁共振(NMR)和二维红外光谱(2D-IR)是研究蛋白质动力学的两种主要方法。在此,我们结合这两种方法,以全新视角理解细胞因子与受体相互作用的复杂机制。如今,许多细胞因子的动态特性被视为信号传导机制中的关键属性。白细胞介素-17(IL-17)是促炎细胞因子,若不受调控,会引发严重的自身免疫性疾病,如银屑病。尽管市场上有多种针对这些病症的疗法,但小分子疗法仍难以寻觅。以往仅利用晶体学方法的研究,无法解释IL-17二聚体与其受体之间观察到的亲和力显著差异,这表明仅通过静态结构分析无法完全解释所有因素。在此,我们表明细胞因子IL-17家族具有不同程度的灵活性,这与其受体亲和力直接相关。细胞因子与受体相互作用的小分子抑制剂通常被认为通过引起空间位阻冲突或结构变化来发挥作用。然而,我们的结果得到了其他生物物理方法的支持,为一种替代抑制机制提供了证据,即小分子使蛋白质刚性化,导致受体亲和力降低。本文呈现的结果表明细胞因子与受体结合的诱导契合模型,即灵活性更高的细胞因子具有更高的亲和力。我们的方法可应用于其他蛋白质 - 蛋白质相互作用抑制难以解决的系统,例如由于界面平坦、缺乏特征。靶向调节蛋白质动力学的变构位点,为新型治疗药物开发开辟了新途径。