ArticleProceedings of the National Academy of Sciences of the United States of America2022
Driving force and pathway in polyelectrolyte complex coacervation.
Article in Proceedings of the National Academy of Sciences of the United States of America, 2022. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 39 papers.
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Who cites it
39 citing papers in PubMed, 105 citations in OpenAlex.
- Biomimetic Coacervate Coatings: From Phase Separation Fundamentals to Advanced Biomedical Applications.Biomimetics (Basel, Switzerland) · 2026Review
- Dynamic and Catalytic Multiphase Coacervates.Biomacromolecules · 2026Article
- Functionalized Coacervates for Cancer Therapy: Advances and Prospects in Phase-Separation-Based Intelligent Drug Delivery.Small (Weinheim an der Bergstrasse, Germany) · 2026Review
- Effect of Copolymer Chemistry on the Humidity- and Temperature-Dependent Mechanical Properties and Structure of Polyelectrolyte Complexes.Macromolecules · 2026Article
- Effect of Polymer Structure on the Thermodynamics of Polyelectrolyte Complex Micelle Formation.Macromolecules · 2026Article
- Decoding nucleic acid contributions to phase separation and ordering in biomolecular condensates.Nucleic acids research · 2026Article
- Mixing protocols determine liquid-liquid phase separation dynamics in polyelectrolyte complex coacervation.Nature communications · 2026Article
- Polymer conformational entropy as the driver of complex coacervation.Proceedings of the National Academy of Sciences of the United States of America · 2026Article
- A unified mechanistic perspective on protein-polysaccharide interactions underlying hybrid gel formation: A mini review.Current research in food science · 2026Review
- Cooperation and Competition of Base Pairing and Electrostatic Interactions in Mixtures of DNA Nanostars and Polylysine.Journal of the American Chemical Society · 2025Article
- Role of Charge Patterning and Hydrophobicity in Peptide-Based Complex Coacervates.Biomacromolecules · 2025Article
- Selective Ion Binding and Uptake Shape the Microenvironment of Biomolecular Condensates.Journal of the American Chemical Society · 2025Article
- Cosolvent Control of Lower and Upper Critical Solution Behavior in Polyelectrolyte Complexes.ACS macro letters · 2025Article
- Tandem-repeat proteins introduce tuneable properties to engineered biomolecular condensates.Chemical science · 2025Article
- Engineering Protein-Polyelectrolyte Interactions for Cellular Applications.Annual review of chemical and biomolecular engineering · 2025Review
- Microstructural Rearrangements in Triblock Polyelectrolyte Complex Hydrogels.ACS macro letters · 2025Article
- Brittle-to-Ductile Transitions of Polyelectrolyte Complexes: Humidity, Temperature, and Salt.Macromolecules · 2025Article
- Network-forming phase separation of oppositely charged polyelectrolytes forming coacervates in a solvent.Nature communications · 2025Article
- Driving Forces in the Formation of Biocondensates of Highly Charged Proteins: A Thermodynamic Analysis of the Binary Complex Formation.Biomolecules · 2024Article
- Unlocking the electrochemical functions of biomolecular condensates.Nature chemical biology · 2024Review
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2 authors at 1 institution in 1 country.
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Abstract
There is notable discrepancy between experiments and coarse-grained model studies regarding the thermodynamic driving force in polyelectrolyte complex coacervation: experiments find the free energy change to be dominated by entropy, while simulations using coarse-grained models with implicit solvent usually report a large, even dominant energetic contribution in systems with weak to intermediate electrostatic strength. Here, using coarse-grained, implicit-solvent molecular dynamics simulation combined with thermodynamic analysis, we study the potential of mean force (PMF) in the two key stages on the coacervation pathway for symmetric polyelectrolyte mixtures: polycation-polyanion complexation and polyion pair-pair condensation. We show that the temperature dependence in the dielectric constant of water gives rise to a substantial entropic contribution in the electrostatic interaction. By accounting for this electrostatic entropy, which is due to solvent reorganization, we find that under common conditions (monovalent ions, room temperature) for aqueous systems, both stages are strongly entropy-driven with negligible or even unfavorable energetic contributions, consistent with experimental results. Furthermore, for weak to intermediate electrostatic strengths, this electrostatic entropy, rather than the counterion-release entropy, is the primary entropy contribution. From the calculated PMF, we find that the supernatant phase consists predominantly of polyion pairs with vanishingly small concentration of bare polyelectrolytes, and we provide an estimate of the spinodal of the supernatant phase. Finally, we show that prior to contact, two neutral polyion pairs weakly attract each other by mutually induced polarization, providing the initial driving force for the fusion of the pairs.
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