This work draws inspiration from nature, specifically the remarkable ability of spiders to manipulate their local environment within the silk gland, enabling the transformation of a proteinaceous solution into a tough silk. This environmental control involves changes in pH, ion type, and ion concentration. Despite being a water-based processing approach, spider silk remains a highly tough and water-insoluble material, offering an environmentally friendly alternative to the more toxic methods currently employed in fiber production.[1]
In this work, we take inspiration from this mechanism by gradually changing the ionic strength of a complex coacervate in a microfluidic chip. Complex coacervation is a form of associative liquid-liquid phase separation driven by electrostatic interactions between oppositely charged (bio-)macromolecules and the release of bound counter-ions, typically resulting in the formation of a polymer dense phase (the coacervate) and a dilute supernatant.[2] Through the modification of the local ionic strength, the physical properties of this coacervate phase can be tuned from a free-flowing viscoelastic fluid to a stiff polyelectrolyte complex.[3] Recent work in our group has provided insights into the effect of the desaltation rate on the porosity of formed complex coacervates, facilitating the creation of highly porous polymeric materials. The goal of this work is to gradually desalt a complex coacervate using microfluidics, allowing for the creation of novel fibrous materials through a green processing approach.
[1] A. Rising and J. Johansson, Nature Chemical Biology 2015, 11, 309-315; b) G. Guessous, L. Blake, A. Bui, Y. Woo and G. Manzanarez, ACS Biomater Sci Eng 2024.
[2] C. E. Sing and S. L. Perry, Soft Matter 2020, 16, 2885-2914.
[3] Q. Wang and J. B. Schlenoff, Macromolecules 2014, 47, 3108-3116.
[4] A. D. Malay, H. C. Craig, J. Chen, N. A. Oktaviani and K. Numata, Biomacromolecules 2022, 23, 1827-1840.