Abstract
The selective removal of trace heteroatomic contaminants from fuel remains a critical challenge for clean combustion and refinery upgrading, particularly due to the chemical stability and structural similarity of sulfur- and nitrogen-containing aromatics. Herein, a surface-engineered graphene oxide aerogel functionalized with cyclodextrin (β-CD-CONH-GO) is developed via covalent grafting to introduce well-defined host-guest recognition sites within a porous framework. Spectroscopic and microscopic characterizations confirm successful functionalization, preserved aerogel morphology, and accessible hybrid interfaces. The removal process for monocyclic, bicyclic, and tricyclic impurities is governed by synergistic molecular inclusion within the cyclodextrin cavity, interfacial hydrogen bonding, and secondary confinement provided by the aerogel porosity. Thus, the β-CD-CONH-GO exhibits efficient adsorption toward representative bicyclic impurities, and the removal performance follows the order of indole > quinoline > benzothiophene. Kinetic analysis demonstrates pseudo-second-order adsorption behavior, indicating chemisorption dominated by cooperative host-guest recognition and hydrogen bonding. It possesses removal selectivity even in mixed systems containing structurally similar aliphatic and aromatic competitors and maintains > 95% efficiency after five regeneration cycles via ethanol extraction, confirming superb durability. This study demonstrates a feasible pathway to design adsorbents for deep fuel refining and highlights cyclodextrin-based graphene hybrid aerogels as promising candidates for separations.