Enhancing Sorbate–Sorbent Interactions via Anchoring Multiple Nitrogen Sites into Multilayered Porous Carbons Enables Superior Toluene Capture

Toluene, a toxic aromatic pollutant widely present in air, poses serious risks to environmental health, especially at trace concentrations. Although porous carbon stands out as one of the most potentially useful materials for toluene capture, achieving superior toluene capture from real-world ambient conditions remains a tough challenge, attributed to weak sorbate–sorbent interactions and competitive adsorption from ubiquitous water vapor. Herein, we propose a design concept centered on driving the tight binding between toluene and sorbent through multiple π–π complexation and point-to-point interactions by anchoring multiple nitrogen sites into multilayered porous carbon (FPC) via a urea-mediated pyrolysis approach. This strong sorbate–sorbent interaction mechanism imparts effectively enhanced adsorption and selectivity for toluene. This behavior enables FPC to achieve a remarkable toluene uptake of 344 mg·g^–1 at trace concentration (400 ppm), surpassing previous benchmarks. More importantly, it maintains 97% efficiency even at 70% relative humidity, a performance unparalleled in known porous carbons. This work demonstrates a practical and scalable approach to designing high-performance carbon adsorbents through molecular-level functionality modulation, providing a feasible solution for the removal of aromatic pollutants under realistic conditions.