Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 58, Issue 50, Pages 18116-18123Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201911782
Keywords
amino acids; liquid-liquid phase separation; nucleation; peptides; supramolecular polymers
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Funding
- National Natural Science Foundation of China [21522307, 21802143, 21773248, 21802144]
- National Natural Science Fund BRICS STI Framework Programme [51861145304]
- Innovation Research Community Science Fund [21821005]
- Key Research Program of Frontier Sciences of the Chinese Academy of Sciences (CAS) [QYZDB-SSW-JSC034]
- UK Biotechnology and Biochemical Sciences Research Council
- European Research Council
- Oppenheimer Early Career Fellowship
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The transition of peptides and proteins from the solution phase into fibrillar structures is a general phenomenon encountered in functional and aberrant biology and is increasingly exploited in soft materials science. However, the fundamental molecular events underpinning the early stages of their assembly and subsequent growth have remained challenging to elucidate. Here, we show that liquid-liquid phase separation into solute-rich and solute-poor phases is a fundamental step leading to the nucleation of supramolecular nanofibrils from molecular building blocks, including peptides and even amphiphilic amino acids. The solute-rich liquid droplets act as nucleation sites, allowing the formation of thermodynamically favorable nanofibrils following Ostwald's step rule. The transition from solution to liquid droplets is entropy driven while the transition from liquid droplets to nanofibrils is mediated by enthalpic interactions and characterized by structural reorganization. These findings shed light on how the nucleation barrier toward the formation of solid phases can be lowered through a kinetic mechanism which proceeds through a metastable liquid phase.
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