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Multifunctionalization of microporous polymers is highly desirable but remains a significant challenge, considering that the current microporous polymers are generally hydrophobic and nonresponsive to different environmental stimuli and difficult to be carbonized without damage of their well-defined nanomorphology. Herein, we demonstrate a facile and versatile method to fabricate water-dispersible, pH/temperature responsive and readily carbonizable hairy microporous polymeric nanospheres based on combination of the hyper-cross-linking chemistry with the surface-initiated atom transfer radical polymerization (SI-ATRP). The hyper-cross-linking creates a highly microporous core, whereas the SI-ATRP provides diverse functionalities by surface grafting of hairy functional blocks. The as-prepared materials present multifunctional properties, including sensitive response to pH/temperature, high adsorption capacity toward adsorbates from aqueous solution, and valuable transformation into well-defined microporous carbon nanospheres because of hybrid of carbonizable core and thermo-decomposable protection shell. We hope this strategy could promote the development of both functional microporous polymers and advanced hairy nanoparticles for multipurpose applications.

Formation of a uniform interface between the carbon precursor and the selected template is critical for preparing high-quality nanoporous carbons. It can be accomplished by various templating procedures but still remains a challenge, especially for microporous carbons. A new strategy to fabricate well-defined microporous carbon nanosphere (MCNS) materials via molecular-scale interfacial engineering using an organic/inorganic hybrid molecule as the building block was designed. A commercially available octaphenyl polyhedral oligomeric silsesquioxane was selected as such a building block and transformed into the MCNS products via cross-linking of organic components, followed by carbonization, and subsequent removal of monodispersed silica domains, surrounded by molecular-scale carbon/silica interfaces. The obtained MCNS materials exhibit very large surface area (e.g., 2264 m(2)/g) and fast and selective sorption, and thus demonstrate excellent adsorption and supercapacitance properties. These findings could provide a new benchmark for preparing well-defined nanoporous carbons for various applications.