4.5 Article

Spatiotemporal control of L-phenylalanine crystallization in microemulsion: the role of water in mediating molecular self-assembly

Journal

IUCRJ
Volume 9, Issue -, Pages 370-377

Publisher

INT UNION CRYSTALLOGRAPHY
DOI: 10.1107/S2052252522003001

Keywords

L-phenylalanine crystallization; microemulsion nanoconfinement; amyloid fibril; self-assembly; morphology; crystal engineering; crystal morphology; polymorphism; pharmaceutical solids

Funding

  1. National Natural Science Foundation of China [21908159]
  2. China Postdoctoral Science Foundation [2019M651039]

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This study investigates the role of water in molecular self-assembly. By using a microemulsion biomimetic system to simulate different water environments, the authors observed the formation of different crystal and fiber structures. The results suggest that different types of water trigger different nucleation and growth pathways.
Water confined or constrained in a cellular environment can exhibit a diverse structural and dynamical role and hence will affect the self-assembly behavior of biomolecules. Herein, the role of water in the formation of L-phenylalanine crystals and amyloid fibrils was investigated. A microemulsion biomimetic system with controllable water pool size was employed to provide a microenvironment with different types of water, which was characterized by small-angle X-ray scattering, attenuated total reflectance- Fourier transform infrared spectroscopy and differential scanning calorimetry. In a bound water environment, only plate-like L-phenylalanine crystals and their aggregates were formed, all of which are anhydrous crystal form I. However, when free water dominated, amyloid fibrils were observed. Free water not only stabilizes new oligomers in the initial nucleation stage but also forms bridged hydrogen bonds to induce vertical stacking to form a fibrous structure. The conformational changes of L-phenylalanine in different environments were detected by NMR. Different types of water trigger different nucleation and growth pathways, providing a new perspective for understanding molecular self-assembly in nanoconfinement.

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