Abstract The development of metal-free catalysts for efficient selective catalytic oxidation of hydrogen sulfide (H 2 S-SCO) to elemental sulfur represents a sustainable solution for toxic gas purification. Herein, we synthesized a regenerable metal-free catalyst through facile activation and pyrolysis of coffee grounds. The optimized catalyst demonstrated exceptional H 2 S-SCO performance at 180 ℃, achieving > 99% H 2 S conversion with near-perfect sulfur selectivity (~ 100%) while maintaining remarkable stability under humid conditions and high CO 2 concentrations. These superior properties originate from the synergistic effects of elevated nitrogen doping (17.33 at.%), abundant defect edge sites, and hierarchical porosity. Density functional theory (DFT) calculations revealed that carbon atoms adjacent to pyridine-N configurations serve as dual-active sites, facilitating H 2 S adsorption/dissociation and O 2 activation through optimized electron redistribution. A plausible reaction mechanism was established based on experimental and theoretical analyses. This work provides fundamental insights into designing cost-effective, biomass-derived carbon catalysts for industrial gas purification while addressing agricultural waste valorization. Graphical Abstract
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