Department of Chemistry and Chemical Biology, Harvard University, Cambridge, Massachusetts; PhD Program in Biophysics, Harvard University, Cambridge, Massachusetts.
Department of Chemistry and Chemical Biology, Harvard University, Cambridge, Massachusetts.
Biophys J. 2023 Aug 22;122(16):3238-3253. doi: 10.1016/j.bpj.2023.07.002. Epub 2023 Jul 7.
Many secreted proteins, including viral proteins, contain multiple disulfide bonds. How disulfide formation is coupled to protein folding in the cell remains poorly understood at the molecular level. Here, we combine experiment and simulation to address this question as it pertains to the SARS-CoV-2 receptor binding domain (RBD). We show that the RBD can only refold reversibly if its native disulfides are present before folding. But in their absence, the RBD spontaneously misfolds into a nonnative, molten-globule-like state that is structurally incompatible with complete disulfide formation and that is highly prone to aggregation. Thus, the RBD native structure represents a metastable state on the protein's energy landscape with reduced disulfides, indicating that nonequilibrium mechanisms are needed to ensure native disulfides form before folding. Our atomistic simulations suggest that this may be achieved via co-translational folding during RBD secretion into the endoplasmic reticulum. Namely, at intermediate translation lengths, native disulfide pairs are predicted to come together with high probability, and thus, under suitable kinetic conditions, this process may lock the protein into its native state and circumvent highly aggregation-prone nonnative intermediates. This detailed molecular picture of the RBD folding landscape may shed light on SARS-CoV-2 pathology and molecular constraints governing SARS-CoV-2 evolution.
许多分泌蛋白,包括病毒蛋白,都含有多个二硫键。在分子水平上,二硫键的形成如何与细胞内的蛋白质折叠偶联仍然知之甚少。在这里,我们结合实验和模拟来解决这个问题,具体来说是针对 SARS-CoV-2 受体结合域(RBD)。我们表明,如果 RBD 在折叠之前存在其天然的二硫键,它只能可逆地重新折叠。但是如果不存在这些二硫键,RBD 会自发错误折叠成一种非天然的、类似无规卷曲的状态,这种状态在结构上与完全形成二硫键不相容,并且非常容易聚集。因此,RBD 的天然结构代表了蛋白质能量景观上的亚稳态,其二硫键减少,表明在折叠之前形成天然二硫键需要非平衡机制。我们的原子模拟表明,这可能是通过 RBD 在内质网分泌过程中的共翻译折叠来实现的。也就是说,在中间翻译长度下,天然的二硫键对很可能以高概率结合在一起,因此,在适当的动力学条件下,这个过程可能会将蛋白质锁定在其天然状态,并避免高度聚集倾向的非天然中间产物。这种对 RBD 折叠景观的详细分子描述可能有助于阐明 SARS-CoV-2 的发病机制和控制 SARS-CoV-2 进化的分子限制。