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Porous Janus Polymer Single Crystals via Liquid-Liquid Phase Separation at Oil-Water Interface
Journal article   Open access   Peer reviewed

Porous Janus Polymer Single Crystals via Liquid-Liquid Phase Separation at Oil-Water Interface

Hao Qi, Shichen Yu and Christopher Y. Li
Giant (Oxford, England), v 29, 100411
Jul 2026
url
https://doi.org/10.1016/j.giant.2026.100411View
Published, Version of Record (VoR) Open

Abstract

Janus nanosheet Liquid-liquid interface Liquid-liquid phase separation Evaporative crystallization Polymer single crystals
Coupling liquid–liquid phase separation (LLPS) with crystallization has emerged as an effective strategy for regulating polymer crystalline structures and elucidating crystallization mechanisms. In this work, we investigate the evaporative crystallization of poly(caprolactone) at water surface using three PCLs with different chain-end functionalities. By tailoring the chain ends and employing evaporative crystallization on water surfaces, the crystallization pathways were systematically controlled, enabling the formation of single-crystalline porous Janus films and two-dimensional (2D) Janus polymer single crystals. The observed structural evolution is attributed to the interplay between LLPS and crystallization during solvent evaporation. These results reveal a strong correlation between polymer chain conformation and crystalline morphology at liquid–liquid interfaces, providing new insights into interfacial polymer crystallization and the design of anisotropic polymeric structures.

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