Three-dimensionally architectured electrochemical energy storage devices enabled by block copolymer-directed functional materials
Carbon-based materials have found widespread use in electrochemical energy storage (EES), due to their favorable properties such as electrical conductivity and high specific surface area. Three-dimensionally continuous nanostructured electrode materials are a field of growing interest, as they present exciting new architectural possibilities for devices. Therefore, the development of nanostructured carbon materials with 3D network architectures and subsequent processing into to 3D functional composite materials is an appealing challenge. Here, ultralarge pore-size carbons with nonperiodically ordered co-continuous network structures and average pore sizes >90 nm were fabricated using ultralarge molar mass poly(styrene-block-2-dimethylaminoethyl methacrylate) linear diblock copolymers as structure-directing agents for phenol-formaldehyde resols carbon precursors. These carbons then had polymer thin film separators uniformly deposited on their surfaces via electropolymerization. Finally, our EES devices were completed via back-filling methods to ubiquitously infiltrate the remaining 3D pore space with both cathode material and current collector. Devices were then connected and electrochemically characterized.