Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 143, Issue 12, Pages 4782-4789Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c01148
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Funding
- German Federal Ministry of Education and Research (BMBF)
- Max Planck Society
- Deutsche Forschungsgemeinschaft via the International Research Training Group ATUMS [IRTG 2022]
- European Research Council (ERC) [852187]
- Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) [364653263 - TRR 235]
- Studienstiftung des deutschen Volkes
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Complex coacervated-based assemblies are formed by the phase separation of two oppositely charged polyelectrolytes, leading to supramolecular architectures with various morphologies. These assemblies have a wide range of applications, including in food industry and medical adhesives, and serve as model systems for biological assemblies. By studying chemically-regulated systems with dynamic maintenance through reaction cycles, researchers aim to develop membraneless organelle models and explore new applications for complex coacervate-based structures.
Complex coacervated-based assemblies form when two oppositely charged polyelectrolytes combine to phase separate into a supramolecular architecture. These architectures range from complex coacervate droplets, spherical and worm-like micelles, to vesicles. These assemblies are widely applied, for example, in the food industry, and as underwater or medical adhesives, but they can also serve as a great model for biological assemblies. Indeed, biology relies on complex coacervation to form so-called membraneless organelles, dynamic and transient droplets formed by the coacervation of nucleic acids and proteins. To regulate their function, membraneless organelles are dynamically maintained by chemical reaction cycles, including phosphorylation and dephosphorylation, but exact mechanisms remain elusive. Recently, some model systems also regulated by chemical reaction cycles have been introduced, but how to design such systems and how molecular design affects their properties is unclear. In this work, we test a series of cationic peptides for their chemically fueled coacervation, and we test how their design can affect the dynamics of assembly and disassembly of the emerging structures. We combine them with both homo- and block copolymers and study the morphologies of the assemblies, including morphological transitions that are driven by the chemical reaction cycle. We deduce heuristic design rules that can be applied to other chemically regulated systems. These rules will help develop membraneless organelle model systems and lead to exciting new applications of complex coacervate-based examples like temporary adhesives.
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