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<p>The development of metal-free catalysts for efficient selective catalytic oxidation of hydrogen sulfide (H<sub>2</sub>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<sub>2</sub>S-SCO performance at 180 ℃, achieving &gt; 99% H<sub>2</sub>S conversion with near-perfect sulfur selectivity (~ 100%) while maintaining remarkable stability under humid conditions and high CO<sub>2</sub> 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<sub>2</sub>S adsorption/dissociation and O<sub>2</sub> 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.</p> Graphical Abstract <p></p>

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Coffee grounds derived porous nitrogen-rich biochar as a metal-free catalyst for efficient selective oxidation of hydrogen sulfide to sulfur

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年1月31日

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  • Fei Zhao,
  • Zibin Pan,
  • Fang Wang,
  • Suo Cui,
  • Rui Cao,
  • Jiayu Feng,
  • Ping Ning,
  • Lijuan Jia

摘要

The development of metal-free catalysts for efficient selective catalytic oxidation of hydrogen sulfide (H2S-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 H2S-SCO performance at 180 ℃, achieving > 99% H2S conversion with near-perfect sulfur selectivity (~ 100%) while maintaining remarkable stability under humid conditions and high CO2 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 H2S adsorption/dissociation and O2 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