Aerobijels: Ultralight Carbon Monoliths from Cocontinuous Emulsions

Bijels are used to develop a new class of ultralight hierarchically porous aerogels exhibiting multimodal porosity across multiple length scales. Through in situ functionalization of a particle‐laden liquid interface wherein binary liquid pairs are kinetically trapped out of equilibrium through interfacial jamming, monolithic and freestanding carbon electrodes are produced with prescribed bulk densities down to ≈2 mg cm^?3. Exemplary electrokinetic experiments indicate that the bicontinuity of the pore structure is essential for enhancing transport to and from the active electrode surfaces, demonstrating that these materials possess a superior ability to accumulate and transport charge when compared to analogous systems with restricted pore connectivity and fluid throughput. This approach offers a new synthetic route to bicontinuous and hierarchical aerogel materials with nested multimodal porosities. The flexibility of this scheme can address critical issues related to transport‐limited behaviors that arise in many technological fields, ranging from energy and catalysis research to remediation and sensing applications.