Polyacrylamide Network Permeation in Hyaluronic Acid and Poly-l-lysine Complex Coacervates

IF 5.7 1区化学 Q1 POLYMER SCIENCE

Macromolecules Pub Date : 2026-10-13 Epub Date: 2026-09-26 DOI:10.1021/acs.macromol.6c00699

Kai R. Yamagami, Ping-Huan Tsai, Charles E. Sing, Svetlana Morozova

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Abstract

For many biomolecular condensates, complex coacervation occurs in a viscoelastic medium, which can permeate the droplets and regulate phase separation. Here, we study the permeation of complex coacervate droplets composed of hyaluronic acid (HA) and poly-l-lysine (PLL) inside synthetic polyacrylamide (PAM) hydrogels (160–2200 Pa). From the confocal images of fluorescently conjugated complex coacervate phases in the background of a separately labeled gel, we measure the intensity-derived normalized gel concentration λ_g. λ_g rose from ∼0.4 in the soft gels to ∼0.6 in the stiffest gels, showing that the extent of permeation is dependent on elasticity. By varying the solvent ionic strength (10–280 mM) and loading polyelectrolyte concentration (2–40 g L^–1), we find that λ_g is maximized near the critical ionic strength and at the lowest polyelectrolyte loading concentration. Straightforward theory is used to explain the overall physical trends, showing that coacervation in a crosslinked network is governed by a competition between network elasticity and excluded volume interactions.

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透明质酸和聚赖氨酸络合物凝聚物中的聚丙烯酰胺网络渗透

摘要对于许多生物分子凝析物，在粘弹性介质中发生复杂的凝聚，可以渗透液滴并调节相分离。在这里，我们研究了透明质酸（HA）和聚赖氨酸（PLL）组成的复杂凝聚液滴在合成聚丙烯酰胺（PAM）水凝胶（160-2200 Pa）中的渗透。在单独标记的凝胶背景下，从荧光共轭络合物凝聚相的共聚焦图像中，我们测量了强度衍生的归一化凝胶浓度λg。λg从软凝胶中的~ 0.4上升到最硬凝胶中的~ 0.6，表明渗透程度取决于弹性。通过改变溶剂离子强度（10-280 mM）和负载聚电解质浓度（2-40 g L-1），我们发现λg在临界离子强度附近和最低负载聚电解质浓度时最大。直接的理论被用来解释整体的物理趋势，表明交联网络中的凝聚是由网络弹性和排除的体积相互作用之间的竞争所控制的。

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来源期刊

Macromolecules 工程技术-高分子科学

CiteScore

9.30

自引率

16.40%

发文量

942

审稿时长

2 months

期刊介绍： Macromolecules publishes original, fundamental, and impactful research on all aspects of polymer science. Topics of interest include synthesis (e.g., controlled polymerizations, polymerization catalysis, post polymerization modification, new monomer structures and polymer architectures, and polymerization mechanisms/kinetics analysis); phase behavior, thermodynamics, dynamic, and ordering/disordering phenomena (e.g., self-assembly, gelation, crystallization, solution/melt/solid-state characteristics); structure and properties (e.g., mechanical and rheological properties, surface/interfacial characteristics, electronic and transport properties); new state of the art characterization (e.g., spectroscopy, scattering, microscopy, rheology), simulation (e.g., Monte Carlo, molecular dynamics, multi-scale/coarse-grained modeling), and theoretical methods. Renewable/sustainable polymers, polymer networks, responsive polymers, electro-, magneto- and opto-active macromolecules, inorganic polymers, charge-transporting polymers (ion-containing, semiconducting, and conducting), nanostructured polymers, and polymer composites are also of interest. Typical papers published in Macromolecules showcase important and innovative concepts, experimental methods/observations, and theoretical/computational approaches that demonstrate a fundamental advance in the understanding of polymers.