Journal
ENVIRONMENTAL SCIENCE & TECHNOLOGY
Volume 48, Issue 17, Pages 10354-10362Publisher
AMER CHEMICAL SOC
DOI: 10.1021/es502585s
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Funding
- National Natural Science Fund of China [21207067, 41372044, 21325731]
- Fundamental Research Funds for the Central Universities [30920130111023]
- Zijin Intelligent Program, Nanjing University of Science and Technology [2013-0106]
- Environmental Scientific Research of Jiangsu Province [2012026]
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The mechanism of N2O formation during the low-temperature selective catalytic reduction reaction (SCR) over Mn-Fe spinel was studied. The in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and transient reaction studies demonstrated that the Eley-Rideal mechanism (i.e., the reaction of adsorbed NH3 species with gaseous NO) and the Langmuir-Hinshelwood mechanism (i.e., the reaction of adsorbed NH3 species with adsorbed NO species) both contributed to N2O formation. However, N2O selectivity of NO reduction over Mn-Fe spine] through the Langmuir-Hinshelwood mechanism was much less than that through the Eley-Rideal mechanism. The ratio of NO reduction over Mn-Fe spinel through the Langmuir-Hinshelwood mechanism remarkably increased; therefore, N2O selectivity of NO reduction over Mn-Fe spinel decreased with the decrease of the gas hourly space velocity (GHSV). As the gaseous NH3 concentration increased, N2O selectivity of NO reduction over Mn-Fe spinel increased because of the promotion of NO reduction through the Eley-Rideal mechanism. Meanwhile, N2O selectivity of NO reduction over Mn-Fe spine] decreased with the increase of the gaseous NO concentration because the formation of NH on Mn-Fe spinel was restrained. Therefore, N2O selectivity of NO reduction over Mn-Fe spinel was related to the GHSV and concentrations of reactants.
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