期刊
ADVANCED MATERIALS
卷 34, 期 20, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202110123
关键词
catalytic oxidation; heterogeneous catalysis; metal-organic frameworks; single-atom catalysis
类别
资金
- National Natural Science Foundation of China [52006073, 21725101, 21521001]
- Natural Science Foundation of Hebei Province of China [E2020502023]
- Fundamental Research Funds for the Central Universities [2020MS104, WK3450000007]
- International Partnership Program of CAS [211134KYSB20190109]
- University of Calgary's Canada First Research Excellence Fund (CFREF) program entitled the Global Research Initiative for Sustainable Low Carbon Unconventional Resources
A new single-atom catalyst Fe-1-N-4-C with excellent catalytic activity and sulfur resistance has been developed for the oxidation of NO and Hg-0, showing promising potential for cleaner coal-fired power plant operations.
Catalytic oxidation of NO and Hg-0 is a crucial step to eliminate multiple pollutants from emissions from coal-fired power plants. However, traditional catalysts exhibit low catalytic activity and poor sulfur resistance due to low activation ability and poor adsorption selectivity. Herein, a single-atom Fe decorated N-doped carbon catalyst (Fe-1-N-4-C), with abundant Fe-1-N-4 sites, based on a Fe-doped metal-organic framework is developed to oxidize NO and Hg-0. The results demonstrate that the Fe-1-N-4-C has ultrahigh catalytic activity for oxidizing NO and Hg-0 at low and room temperature. More importantly, Fe-1-N-4-C exhibits robust sulfur resistance as it preferably adsorbs reactants over sulfur oxides, which has never been achieved before with traditional catalysts. Furthermore, SO2 boosts the catalytic oxidation of NO over Fe-1-N-4-C through accelerating the circulation of active sites. Density functional theory calculations reveal that the Fe-1-N-4 active sites result in a low energy barrier and high adsorption selectivity, providing detailed molecular-level understanding for its excellent catalytic performance. This is the first report on NO and Hg-0 oxidation over single-atom catalysts with strong sulfur tolerance. The outcomes demonstrate that single-atom catalysts are promising candidates for catalytic oxidation of NO and Hg-0 enabling cleaner coal-fired power plant operations.
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