Multistep Desolvation as a Fundamental Principle Governing Peptide Self-Assembly Through Liquid-Liquid Phase Separation  

作　　者：Chengqian Yuan Ruirui Xing Jie Cui Wei Fan Junbai Li Xuehai Yan 

机构地区：[1]State Key Laboratory of Biochemical Engineering,Institute of Process Engineering,Chinese Academy of Sciences,Beijing 100190 [2]School of Chemical Engineering,University of Chinese Academy of Sciences,Beijing 100049 [3]Analysis and Test Center,Institute of Chemistry,Chinese Academy of Sciences,Beijing 100190 [4]Beijing National Laboratory for Molecular Sciences,CAS Key Laboratory of Colloid,Interface and Chemical Thermodynamics,Institute of Chemistry,Chinese Academy of Sciences,Beijing 100190 [5]Center for Mesoscience,Institute of Process Engineering,Chinese Academy of Sciences,Beijing 100190

出　　处：《CCS Chemistry》2024年第1期255-265,共11页中国化学会会刊（英文）

基　　金：supported by the National Science Fund for Distinguished Young Scholars of China(grant no.22025207);National Natural Science Foundation of China(grant nos.22172172 and 22232006);Youth Innovation Promotion Association of CAS(grant no.2022049);China Scholarship Council(CSC,grant no.202104910187);IPE Project for Frontier Basic Research(grant no.QYJC-2022-011);Natural Science Foundation of Hebei Province(grant nos.B2020103036 and B2020103025).

摘　　要：Biomolecular self-assembly based on peptides and proteins is a general phenomenon encountered in natural and synthetic systems.Liquid–liquid phase separation(LLPS)is intimately involved in biomolecular self-assembly,yet the key factors at a molecular scale activating or modulating such a process remain largely elusive.Herein,we discovered in our experiments that multistep desolvation is fundamental to the formation and evolution of peptide-rich droplets:The first step was partial desolvation of peptides to form peptide clusters,and the second step was selective desolvation of hydrophobic groups within clusters to trigger LLPS and the formation of peptiderich droplets,followed by complete desolvation of droplets,initiating the nucleation of peptide selfassembly.Manipulation of the degree of desolvation at different stages was an effective strategy to control the self-assembly pathways and polymorphisms.This study sheds light on the molecular origin of LLPS-mediated self-assembly distinct from classical one-step self-assembly and paves the way for the precise control of supramolecular self-assembly.

关 键 词：PEPTIDE liquid-liquid phase separation multistep desolvation NANOSTRUCTURES SELF-ASSEMBLY 

分 类 号：O65[理学—分析化学]