Department of Chemistry, King's College London, Britannia House, 7 Trinity Street, London SE1 1DB, UK.
Department of Chemistry, University of Bath, 1 South Building, Claverton Down, Bath BA2 7AY, UK.
J Chem Inf Model. 2022 May 23;62(10):2481-2489. doi: 10.1021/acs.jcim.1c01441. Epub 2022 May 3.
Transient receptor potential (TRP) ion channels are important pharmacological targets because of their role in the perception of pain, and so, understanding their chemical regulation is essential for the development of analgesic drugs. Among the currently known TRP channel chemical agonists, capsaicin, the active compound of chili pepper, is probably the most exhaustively studied. The availability of the three-dimensional structure of the vanilloid receptor 1 (TRPV1) has fueled computational studies revealing the molecular details of capsaicin binding modes. Although this is a significant step, a comprehensible binding mechanism or pathway is invaluable for targeting TRP channels in modern pharmacology. In the present work, free-energy and enhanced sampling techniques have been used to explore a possible membrane-mediated pathway for capsaicin to enter the TRPV1 binding pocket where capsaicin accesses the protein starting at the extracellular milieu through the outer leaflet and into its binding site in the protein. The main states visited along this route have been characterized and include (i) a bound state in agreement with the binding mode "head-down, tail-up" and (ii) an alternative state corresponding to a "head-up, tail-down" binding mode. In agreement with previous reports, binding is mediated by both hydrogen bonds and van der Waals interactions, and residue Y511 is crucial for stabilizing the bound state and during the binding process. Together, these results provide a foundation to further understand TRPV channels, and they could be used to guide therapeutic design of selective inhibitors potentially leading to novel avenues for pharmacological applications targeting the TRPV1 channel.
瞬时受体电位 (TRP) 离子通道是重要的药理学靶点,因为它们在疼痛感知中发挥作用,因此,了解它们的化学调节对于开发镇痛药至关重要。在目前已知的 TRP 通道化学激动剂中,辣椒素是辣椒的活性化合物,可能是研究最彻底的。香草素受体 1 (TRPV1) 的三维结构的可用性激发了计算研究,揭示了辣椒素结合模式的分子细节。尽管这是一个重要的步骤,但对于现代药理学中靶向 TRP 通道而言,可理解的结合机制或途径是无价的。在目前的工作中,使用自由能和增强采样技术来探索辣椒素进入 TRPV1 结合口袋的可能膜介导途径,其中辣椒素从细胞外环境开始通过外叶层进入蛋白质,并进入其在蛋白质中的结合位点。沿着这条路线访问的主要状态已被表征,包括 (i) 与“头朝下,尾朝上”结合模式一致的结合状态和 (ii) 对应于“头朝上,尾朝下”结合模式的替代状态。与之前的报告一致,结合由氢键和范德华相互作用介导,并且残基 Y511 对于稳定结合状态和结合过程至关重要。总之,这些结果为进一步了解 TRPV 通道提供了基础,并且可以用于指导潜在的选择性抑制剂的治疗设计,从而为靶向 TRPV1 通道的药理学应用开辟新途径。