Computational Pharmacy, Department of Pharmaceutical Sciences, University of Basel, Klingelbergstrasse 61, Basel 4056, Switzerland.
J Chem Inf Model. 2021 Feb 22;61(2):1010-1019. doi: 10.1021/acs.jcim.0c01403. Epub 2021 Jan 15.
Thyroid hormone receptors (TRs) play a critical role in human development, growth, and metabolism. Antagonists of TRs offer an attractive strategy to treat hyperthyroidism without the disadvantage of a delayed onset of drug action. While it is challenging to examine the atomistic behavior of TRs in a laboratory setting, computational methods such as molecular dynamics (MD) simulations have proven their value to elucidate ligand-induced conformational changes in nuclear receptors. Here, we performed MD simulations of TRα and TRβ complexed to their native ligand triiodothyronine (T3) as well as several antagonists. Based on the examination of 27 μs MD trajectories, we showed how binding of these compounds influences various structural features of the receptors including the helicity of helices 3 and 10 as well as the location of helix-12. Helices 3 and 12 are known to mediate coactivator association required for downstream signaling, suggesting these changes to be the molecular basis for TR antagonism. A mechanistic analysis of the trajectories revealed an allosteric pathway between H3 and H12 to be responsible for the conformational adaptations. Even though a mechanistic understanding of conformational adaptations triggered by TR antagonists is important for the development of novel therapeutics, they have not been previously examined in detail as it was done here.
甲状腺激素受体 (TRs) 在人类的发育、生长和代谢中起着至关重要的作用。TRs 的拮抗剂为治疗甲状腺功能亢进症提供了一种有吸引力的策略,而没有药物作用延迟的缺点。虽然在实验室环境中检查 TRs 的原子行为具有挑战性,但分子动力学 (MD) 模拟等计算方法已被证明可用于阐明核受体中配体诱导的构象变化。在这里,我们对与天然配体三碘甲状腺原氨酸 (T3) 以及几种拮抗剂结合的 TRα 和 TRβ 进行了 MD 模拟。基于对 27 μs MD 轨迹的检查,我们展示了这些化合物的结合如何影响受体的各种结构特征,包括螺旋 3 和 10 的螺旋性以及螺旋 12 的位置。众所周知,螺旋 3 和 12 介导了下游信号传导所需的共激活因子的结合,这表明这些变化是 TR 拮抗作用的分子基础。轨迹的机制分析揭示了 H3 和 H12 之间的变构途径是导致构象适应的原因。尽管了解 TR 拮抗剂触发的构象适应的机制对于开发新的治疗方法很重要,但它们以前没有像这里那样进行详细检查。