Chemically Programmable Liquid-to-Solid Transitions and Spatial Dynamics in Synthetic Coacervates.

Authors

Zixuan Wu, Mengyue Zhu, Peiyong Song, Zhetong Liu, Jianming Li, Rong Huang, Yan Qiao, Yiyang Lin

Published in

Journal of the American Chemical Society. Jul 01, 2026. Epub Jul 01, 2026.

Abstract

Biomolecular condensates undergo dynamic maturation, transitioning from liquid-like droplets to gel-like or solid-like assemblies, exhibiting structural heterogeneity in response to biochemical cues. Synthetic coacervate droplets formed via liquid-liquid phase separation (LLPS) have emerged as simplified models of these condensates and of protocells. Yet, the understanding of complex phase behaviors of liquid-like droplets in both biological and chemical contexts remains less explored, limiting our understanding of biological function and the design of droplet-based soft materials and protocells. Here, we introduce a chemically programmable strategy to dynamically modulate droplet phase transitions through controlled polymer-network cross-linking. Reactive cross-linkers selectively engage polymers within liquid-like droplets, progressively increasing internal microviscosity and inducing a liquid-to-solid transition. Beyond uniform phase regulation, network cross-linking drives spatially heterogeneous phase separation via polymer demixing and Ostwald ripening, with reaction-diffusion dynamics critically shaping both thermodynamically stable and metastable droplets. Using orthogonal cleavable cross-linkers, we further demonstrate chemical control over droplet liquefaction and the generation of multiphasic structures with pathway-dependent configurations. Integration of photoresponsive cross-linkers with digital-micromirror device (DMD) technology enables precise spatial photopatterning of droplet networks. This work establishes a versatile framework for elucidating the structural principles of microphase separation within coacervates and provides a blueprint for designing dynamic soft materials and synthetic protocells.

PMID:
42387255
Bibliographic data and abstract were imported from PubMed on 02 Jul 2026.

Read full publication at:
Please sign in to see all details.

Stats

1-terrible, 9-excellent. How would you rate this publication? Sign in in to submit your rating.

Post a comment

You need to be signed in to post comments. You can sign in here.

Comments

There are no comments yet.