4.5 Article

Insight into N2O Formation Over Different Crystal Phases of MnO2 During Low-Temperature NH3-SCR of NO

Journal

CATALYSIS LETTERS
Volume 151, Issue 10, Pages 2964-2971

Publisher

SPRINGER
DOI: 10.1007/s10562-021-03541-8

Keywords

MnO2; Different crystal phases; NH3-SCR; N2O formation

Funding

  1. National Natural Science Foundation of China [51874058]
  2. Chongqing Talents Plan for Young Talents [CQYC201905017]
  3. Graduate Research and Innovation Foundation of Chongqing, China [CYB20003]
  4. Fund of Chongqing Science and Technology [cstc2019jscx-msxmX0215, cstc2019jscx-fxydX0009]

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Different crystal phases of MnO2 were synthesized and tested for NH3-SCR of NO and NH3 oxidation performances, showing varying reactivities towards oxygen and NH3 species on the catalyst surfaces. Alpha-MnO2 exhibited superior SCR performance for NOx conversion, while beta-MnO2 showed lower reactivity for N2O production due to NH3 adsorbed at Lewis sites. Gamma-MnO2 yielded similar NOx conversion rates as alpha-MnO2 but produced more N2O from SCR reactions. Delta-MnO2 mainly generated N2O from SCR reactions and had difficulty reacting with O-2.
Different crystal phases of MnO2 were synthesized and tested for NH3-SCR of NO and NH3 oxidation performances during 50-120 degrees C. Among those catalysts, alpha-MnO2 showed the most superior SCR performance for NOx conversion and N-2 selectivity, and NH3 species on its surface were active to react with the oxygen, while NH2 species were also easily oxidized by the oxygen. For beta-MnO2, NH3 (ads, B) species and part of NH3 (ads, L) species on its surface were active to react with oxygen, while NH3 (ads, L) species adsorbed at Lewis sites showed low reactive with O-2, thereby producing less N2O and low NO conversion. gamma-MnO2 showed the similar NOx conversion rates and N2O amount generated from the NH3 oxidation comparing to alpha-MnO2, while yielding much more N2O generation ratios from SCR reactions conditions. Besides, NH3 (ads, L), NH3 (ads, B), NO32- and NH2 species adsorbed on gamma-MnO2 surface had high reactivity and could all be consumed by oxygen rapidly. And the N2O formation of delta-MnO2 mainly generated from SCR reactions conditions in the temperature range of 50-120 degrees C, while the adsorbed NH3 (ads, L) species were hard to react with O-2. [GRAPHICS]

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