4.8 Article

Reaction Pathway Investigation on the Selective Catalytic Reduction of NO with NH3 over Cu/SSZ-13 at Low Temperatures

Journal

ENVIRONMENTAL SCIENCE & TECHNOLOGY
Volume 49, Issue 1, Pages 467-473

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/es503430w

Keywords

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Funding

  1. National Natural Science Fund of China [21325731, 51478241]
  2. National High-Tech Research and Development (863) Program of China [2013AA065304]
  3. Jiangsu Specially-Appointed Professor Program [R2012T01]
  4. Ford China University Research Program from the Chemical Engineering & Fuel Cell department, Research & Innovation Center, Ford Motor Company

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The mechanism of the selective catalytic reduction of NO with NH3 was studied using Cu/SSZ-13. The adspecies of NO and NH3 as well as the active intermediates were investigated using in situ diffuse reflectance infrared Fourier transform spectroscopy and temperature-programmed surface reaction. The results revealed that three reactions were possible between adsorbed NH3 and NOx. NO2- could be generated by direct formation or NO3- reduction via NO. In a standard selective catalytic reduction (SCR) reaction, NO3- was hard to form, because NO2- was consumed by ammonia before it could be further oxidized to nitrates. Additionally, adsorbed NH3 on the Lewis acid site was more active than NH4+. Thus, SCR mainly followed the reaction between Lewis acid site-adsorbed NH3 and directly formed NO2-. Higher Cu loading could favor the formation of active Cu-NH3, Cu-NO2-, and Cu-NO3-, improving the SCR activity at low temperature.

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