Robust and Flexible Carbon Nanofibers Doped with Amine Functionalized Carbon Nanotubes for Efficient CO₂ Capture

Porous carbon nanofibrous materials have great potential for energy‐efficient CO₂ capture and separations, but a major hurdle is the lack of mechanical strength and flexibility. Herein, the authors report a facile strategy for the fabrication of amine functionalized carbon nanotube (NC) doped carbon nanofibers (CNFs) (denoted as NC@CNFs) with high flexibility and hierarchical porosity. The NC@CNFs are used as robust fibrous adsorption materials for CO₂ capture, which achieve superior CO₂ uptake of 6.3 mmol g⁻¹ at 1.0 bar and 298 K, as well as remarkable CO₂/N₂ selectivity and excellent cyclability. Integrating NC into CNFs not only brings number of adsorption sites (i.e., NH₂) and tunable hierarchical pores for CO₂ uptake, but also serves as single‐fiber‐crack connection to prevent NC@CNFs from brittle fracture. More significantly, the flexible NC@CNFs with highly stable structure and mechanical strength can overcome the limitation of easy pulverization and structure collapses for traditional particle‐shaped solid sorbents, which makes them highly operable and applicable. This work paves the way for a new route to produce fibrous textile materials with high flexibility and outstanding performance for gas separation.