The Role of Chemically Innocent Polyanions in Active,Chemically Fueled Complex Coacervate Droplets |
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Authors: | Fabian Späth Anton S Maier Michele Stasi Alexander M Bergmann Kerstin Halama Monika Wenisch Bernhard Rieger Job Boekhoven |
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Institution: | 1. Department of Chemistry, School of Natural Sciences, Technical University of Munich, Lichtenbergstrasse 4, 85748 Garching, Germany;2. WACKER-Chair of Macromolecular Chemistry, Catalysis Research Center, Technical University of Munich, Lichtenbergstrasse 4, 85748 Garching, Germany |
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Abstract: | Complex coacervation describes the liquid-liquid phase separation of oppositely charged polymers. Active coacervates are droplets in which one of the electrolyte's affinity is regulated by chemical reactions. These droplets are particularly interesting because they are tightly regulated by reaction kinetics. For example, they serve as a model for membraneless organelles that are also often regulated by biochemical transformations such as post-translational modifications. They are also a great protocell model or could be used to synthesize life–they spontaneously emerge in response to reagents, compete, and decay when all nutrients have been consumed. However, the role of the unreactive building blocks, e.g., the polymeric compounds, is poorly understood. Here, we show the important role of the chemically innocent, unreactive polyanion of our chemically fueled coacervation droplets. We show that the polyanion drastically influences the resulting droplets′ life cycle without influencing the chemical reaction cycle–either they are very dynamic or have a delayed dissolution. Additionally, we derive a mechanistic understanding of our observations and show how additives and rational polymer design help to create the desired coacervate emulsion life cycles. |
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Keywords: | Chemically Fueled Coacervation Membraneless Organelles Peptides Polyelectrolytes Protocells |
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