Innovative Design Strategies for Developing Self-Assembling Hierarchical Porous Materials for Low-Carbon Applications

Hierarchically porous structured materials with multifunctional properties and higher order dimensional complexities are highly desirable for various sustainable energy and environmental applications. This contribution explores our recent advancements in synthesizing hierarchical porous polymeric and inorganic structures for low-carbon applications, using commercial thermoplastic copolymers in directed self-assembly processes that operate under both thermodynamic equilibrium and far-from-equilibrium conditions. We have employed additive selection to precisely control the formation of mesoscale and macroscale structure order and porosity within the resulting hierarchical polymeric and inorganic carbon and oxide structures. Additionally, our use of solvent chemistry has accelerated the simultaneous polymerization of oligomeric modifying agents and the spinodal decomposition-induced phase separation, resulting in electrically conductive and mechanically flexible polymer and carbon porous structures. By coupling copolymer self-assembly with transient annealing, we have effectively regulated atomic and molecular diffusivities and supercooling kinetics, enabling the precise generation of well-defined nanostructures ranging from single atoms to nanoparticles, as well as thin films and bulk solids. These self-assembly-derived hierarchical porous materials are fundamentally and technologically vital for emerging low-carbon technologies, including carbon dioxide adsorbents, separation processes, energy storage, and water splitting.