Phase Separation via Controlled Chain-Growth to Tailor Bicontinuous Monoliths

Bicontinuous structures, which occur across length-scales from nanometers to centimeters, are found throughout nature, and phase separation is a critical process in forming these precise and intricate morphologies. The ability to synthetically create bicontinuous structures is highly sought after due to their potential applications in catalysis, filtration, photonics, and mechanical systems. Recently, a technique known as Elastic Microphase Separation (EMPS) has enabled the production of bicontinuous structures with precise spatial control through phase separation within an elastic network. In this work, we present the development of Polymerization-Induced Elastic Microphase Separation (PI-EMPS), a novel method for initiating phase separation through a controlled chain-growth polymerization strategy. We demonstrate how PI-EMPS facilitates the creation of bicontinuous monoliths from various monomeric liquid phases, with network architecture and extent of polymerization playing key roles in controlling the feature length-scales. Additionally, we describe a technique for selectively depolymerizing the elastic matrix, enabling the isolation and removal of the bicontinuous monolith. This approach opens avenues for producing materials with diverse morphologies tailored to a range of advanced applications.