General Formation of Macro‐/Mesoporous Nanoshells from Interfacial Assembly of Irregular Mesostructured Nanounits

Mesoporous core-shell nanostructures holding controllable ultra-large open channels in their nanoshells are of great interests for the development of new catalytic platforms, electrochemical energy systems, and biological macromolecular carriers. However, soft template-directed cooperative assembly to mesoporous nanoshells with highly accessible pores larger than 30 nm, or even above 50 nm into macroporous range, remains a significant challenge. Herein we report a general approach for precisely tailored coating of hierarchically macro-/mesoporous polymer and carbon shells, possessing highly accessible radial channels with extremely wide pore size distribution from ~10 nm to ~200 nm, on diverse functional materials. This strategy creates opportunities to tailor the interfacial assembly of irregular mesostructured nanounits on core materials and generate various core-shell nanomaterials with controllable pore architectures. Lastly, we confirm that the obtained Fe,N-doped macro-/mesoporous carbon nanoshells show enhanced electrochemical performance for oxygen reduction reaction in alkaline condition.