Insight into synergistic effects of oxygen and nitrogen dual-dopants in carbon catalysts on selective catalytic reduction of NOx with NH3: A combined computational and experimental verification
Chemical Engineering Journal(2023)
摘要
Heteroatom doping in carbon catalysts has been shown to enhance the low-temperature selective catalytic reduction of NOx with NH3 (NH3-SCR); however, precise identification of active structure and activity origin remains challenging as various heteroatoms co-existence. Here, we provide a new insight into the synergistic effects of oxygen and nitrogen dual-dopants on carbon-catalyzed NH3-SCR. Density functional theory calculations reveal a new reaction pathway that the quaternary N enhances O-2 activation and NO oxidation, and carboxyl as Bronsted acid site coupling H2O as H mediator decreases energy barriers of intermediate NH2NO evolution by enhancing H transfer, which was further experimentally verified by model activated cokes with controllable doping patterns. The dual-doped activated coke delivers superior NO conversion (similar to 90 %) and N-2 selectivity (above 90 %) with H2O presence and corresponding kinetic and in-situ characterizations evidence the reaction pathway on dual-doped carbon. This work guides the design of high-performance heteroatom doped carbon catalysts for NH3-SCR.
更多查看译文
关键词
Selective catalytic reduction,Carbon catalyst,Nitrogen and oxygen dual-dopants,Synergistic effect,Density functional theory
AI 理解论文
溯源树
样例
![](https://originalfileserver.aminer.cn/sys/aminer/pubs/mrt_preview.jpeg)
生成溯源树,研究论文发展脉络
Chat Paper
正在生成论文摘要