Tunable Hierarchically Structured Meso-Macroporous Carbon Spheres from a Solvent-Mediated Polymerization-Induced Self-Assembly

Herein, we report a versatile solvent-mediated polymerization-induced self-assembly (PISA) strategy to directly synthesize highly N-doped hierarchically porous structured carbon spheres with a tunable meso-macroporous configuration. The introduction of intermolecular hydrogen bonds is verified to enhance the interfacial interactions between block copolymers, oil droplets, and polyphenols. Moreover, the dominant hydrogen-bond-driven interactions can be systematically manipulated by selecting different cosolvent systems to generate diverse porous structures from the transformation of micellar and precursor co-assembly. Impressively, hierarchically structured meso-macroporous N-doped carbon spheres present simultaneously tunable sphere sizes and mesopores and macropores, ranging from 1.2 μm, 9/50 and 227 nm to 1.0 μm, 40, and 183 nm and 480, 24, and 95 nm. As a demonstration, dendritic-like N-doped hierarchically meso-macroporous carbon spheres manifest excellent enzyme-like activity, which is attributed to the continuous mass transport from the multiordered porosity. The current study provides a new platform for the synthesis of novel well-defined porous materials.