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Regulating Electron Metal–Support Interaction to Suppress N<sub>2</sub>O Formation in the Selective Catalytic Oxidation of Ammonia

Yan Zhang, Meng Wang, Qing Li, Min Zhang, Caixia Liu, Qingling Liu, Weichao Wang, Ziyin Zhang, Rui Han, Na Ji

2023Environmental Science & Technology20 citationsDOI

Abstract

N 2 O is a common byproduct in the selective catalytic oxidation of ammonia, and its generation often needs to be inhibited due to its strong greenhouse effect. In this paper, using Ag/ZSO-Y as a model catalyst, the N 2 O selectivity was reduced by 30% through modulation of the electron metal–support interaction. The results demonstrate that the work function of the support can be regulated by the content of the doping element. As the Zr content increases in SnO 2, the work function of the support decreases. Moreover, there is a positive correlation between the charge transfer amount and the work function of the support. A series of in situ DRIFTS and density functional theory calculations revealed that the –NO and –N reactions are the primary pathways for N 2 O formation. By adjustment of the work function of the support through varying the Zr doping level, the electronic structure of Ag NPs was further tuned, resulting in an increased reaction energy barrier for –NO and –N reactions, effectively suppressing N 2 O formation.

Topics & Concepts

CatalysisWork functionAmmoniaMetalChemistryElectron transferWork (physics)DopingSelectivityInorganic chemistryDensity functional theoryRedoxChemical engineeringMaterials sciencePhotochemistryComputational chemistryThermodynamicsOrganic chemistryEngineeringOptoelectronicsPhysicsCatalytic Processes in Materials ScienceAmmonia Synthesis and Nitrogen ReductionAdvanced Photocatalysis Techniques
Regulating Electron Metal–Support Interaction to Suppress N<sub>2</sub>O Formation in the Selective Catalytic Oxidation of Ammonia | Litcius