Abstract

The development of membrane-based materials that exhibit the range and robustness of autonomic functions found in biological systems remains elusive. Droplet interface bilayers (DIBs) have been proposed as building blocks for such materials, owing to their simplicity, geometry, and capability for replicating cellular phenomena. Similar to how individual cells operate together to perform complex tasks and functions in tissues, networks of functionalized DIBs have been assembled in modular/scalable networks. Here we present the printing of different configurations of picoliter aqueous droplets in a bath of thermoreversible organogel consisting of hexadecane and SEBS triblock copolymers. The droplets are connected by means of lipid bilayers, creating a network of aqueous subcompartments capable of communicating and hosting various types of chemicals and biomolecules. Upon cooling, the encapsulating organogel solidifies to form self-supported liquid-in-gel, tissue-like materials that are robust and durable. To test the biomolecular networks, we functionalized the network with alamethicin peptides and alpha-hemolysin (αHL) channels. Both channels responded to external voltage inputs, indicating the assembly process does not damage the biomolecules. Moreover, we show that the membrane properties may be regulated through the deformation of the surrounding gel.

Highlights

  • The Droplet interface bilayers (DIBs) consists of a lipid bilayer formed at the interface of two lipid-encased aqueous droplets in oil[8,10,16]

  • SEBS is selected as the support for the DIB networks due to its stability and resilience to degradation compared to other types of polymers[34,35]

  • Previous studies with SEBS primarily used a 10 mg/mL concentration of the polymer in the oil phase to improve the durability of the DIB networks[31], but a greater gel stiffness is required for self-supporting structures and for regulating membrane dimensions through compression of the gel

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Summary

Introduction

The DIB consists of a lipid bilayer formed at the interface of two lipid-encased aqueous droplets in oil[8,10,16]. Venkatesan et al addressed this challenge by stabilizing the hexadecane-based oil phase with low concentrations of Poly(styrene-b-ethylene-co-butylene-b-styrene) (SEBS), a thermosensitive copolymer, creating soft liquid-in-gel systems for single DIBs31. They proved that this method successfully improved the portability and durability of the bilayer system without affecting the bilayer’s properties or its ability to host transmembrane peptides such as alamathecin. We combine the mechanical properties of organogels with the versatile functionalities offered by network of bilayer membranes to create a self-supporting, solid material composite with stimuli-responsive capabilities. We optimized the properties of the organogel for our developed manufacturing process to rapidly create and solidify biomolecular networks

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