Single-atom iron as a promising low-temperature catalyst for selective catalytic reduction of NOx with NH3: A theoretical prediction

[Display omitted] •A novel single atom iron catalyst for NH3-SCR.•Environmentally friendly Fe1-N4 with high low-temperature efficiency.•Reaction mechanism in atomic level and microkinetic modeling. Selective catalytic reduction of NOx with NH3 (NH3-SCR) is a dominant technology to reduce NOx (deNOx)...

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Bibliographic Details
Published in:Fuel (Guildford) 2021-10, Vol.302, p.1, Article 121041
Main Authors: Yang, Weijie, Ren, Jianuo, Zhang, Hanwen, Li, Jiajia, Wu, Chongchong, Gates, Ian D., Gao, Zhengyang
Format: Article
Language:English
Subjects:
Ammonia
Catalysts
Chemical reduction
Density functional theory
DFT calculation
Intermediates
Iron
Kinetic analysis
Low temperature
Metal oxides
Microkinetic modeling
NH3-SCR
Nitrogen dioxide
Nitrogen oxides
Oxidation
Oxides
Reaction mechanisms
Selective catalytic reduction
Single-atom catalyst
Thermodynamic analysis
Titanium
Toxicity
Vanadium
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Summary:[Display omitted] •A novel single atom iron catalyst for NH3-SCR.•Environmentally friendly Fe1-N4 with high low-temperature efficiency.•Reaction mechanism in atomic level and microkinetic modeling. Selective catalytic reduction of NOx with NH3 (NH3-SCR) is a dominant technology to reduce NOx (deNOx). However, there are two shortcomings for commercial deNOx catalysts (vanadium-titanium-based metal oxides), such as poor low-temperature efficiency and toxicity. Thus, it is urgent to develop environmentally friendly low-temperature catalysts with high deNOx efficiency. Therefore, we firstly proposed a single-atom iron coordinated with four N atoms (Fe1-N4) as a novel low-temperature NH3-SCR catalyst, due to its high coordination unsaturation and safety. The detailed reaction mechanisms are revealed via density functional theory calculations and microkinetic modeling. Seven possible reaction pathways were found in the NH3-SCR reaction. Different from metal oxides, special intermediates such as N2H and NHNO are found in the reaction pathway. The dominant pathway of the NH3-SCR reaction over the Fe1-N4 catalyst is a three-step process including NO oxidation, NO2 reduction, and NHNO decomposition. The suitable temperature window of the Fe1-N4 catalyst is
ISSN:0016-2361
1873-7153
DOI:10.1016/j.fuel.2021.121041