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Abstract:
Developing efficient strategies for converting hazardous hydrogen sulfide (H2S) waste into valuable products is crucial for mitigating environmental pollution and maximizing resource utilization. Herein, we present a novel approach for the selective reduction of nitroarenes (PhNO2) to arylamines (PhNH2) utilizing H2S as the hydrogen source. This process is facilitated by isolated Fe-Nx sites embedded within graphitic carbon nitride (Fe-CN-x) obtained through a polymerization assembly method. The Fe-CN-3 catalyst, in particular, achieves PhNO2 conversion of 92.0 % with PhNH2 selectivity of 95.8 % at 110°C within 2 h reaction, outperforming the Bulk-CN, commercial active carbon, and commercial Fe2O3. Furthermore, the Fe-CN-3 catalyst can further trigger the reduction of other substituted PhNO2 with high activities. Importantly, the Fe-CN-3 catalyst is resistant to sulfur poisoning, exhibiting high durability, with no obvious decline of catalytic activity in five cycles. Systematic characterizations and density functional theory calculation (DFT) disclose that the isolated Fe atoms prefer to occupy four-coordinate doping configurations (Fe-N4) and the key to this mechanism is the hydrogen transfer process from PhNHOH* + HS* → PhNH* + S + H2O. © 2025 Elsevier B.V.
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Chemical Engineering Journal
ISSN: 1385-8947
Year: 2025
Volume: 512
1 3 . 4 0 0
JCR@2023
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ESI Highly Cited Papers on the List: 0 Unfold All
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30 Days PV: 4
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