Engineering of Microcage Carbon Nanotube Architectures with Decoupled Multimodal Porosity and Amplified Catalytic Performance

New approaches for the engineering of 3D microstructure, pore modality, and chemical functionality hierarchically porous nanocarbon assemblies are key to develop next generation functional aerogel membrane materials. Here, interfacially driven assembly carbon nanotubes (CNT) is exploited fabricate structurally directed aerogels with highly controlled internal architectures, composed pseudo-monolayer, CNT microcages. Pickering emulsions enable at fundamentally different length scales, whereby microporosity, mesoporosity, macroporosity decoupled individually through type, number density, process energy, respectively. In addition, metal nanocatalysts (Cu, Pd, Ru) embedded within architectures an elegant sublimation shock-decomposition approach; introducing first approach that enables through-volume functionalization intricate, pre-designed without microstructural degradation. Catalytic structure–function relationships explored in a pharma-important amidation reaction; providing insights on how engineered frameworks enhance catalyst activity. A sophisticated array advanced tomographic, spectroscopic, microscopic techniques reveal intricate building-blocks their influence properties enhanced nanocatalysts. These advances set basis modulate structure chemistry materials independently fashion variety applications, including energy conversion storage, smart electronics, (electro)catalysis.