We describe fabrication of three-dimensional (3D) multifunctional nanoarchitectures in which the three critical components of a battery—cathode, separator/electrolyte, and anode—are internally assembled as tricontinuous nanoscopic phases. The architecture is initiated using sol–gel chemistry and processing to erect a 3D self-wired nanoparticulate scaffold of manganese oxide (>200 m2 g−1) with a continuous, open, and mesoporous void volume. The integrated 3D system is generated by exhaustive coverage of the oxide network by an ultrathin, conformal layer of insulating polymer that forms via self-limiting electrodeposition of poly(phenylene oxide). The remaining interconnected void volume is then wired with RuO2 nanowebs using subambient thermal decomposition of RuO4. Transmission electron microscopy demonstrates that the three nanoscopic charge-transfer functional components—manganese oxide, polymer separator/cation conductor, and RuO2—exhibit the stratified, tricontinuous design of the phase-by-phase construction. This architecture contains all three components required for a solid-state energy storage device within a void volume sized at tens of nanometres such that nanometre-thick distances are established between the opposing electrodes. We have now demonstrated the ability to assemble multifunctional energy-storage nanoarchitectures on the nanoscale and in three dimensions.
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