Molecular-Level Insight into Selective Catalytic Reduction of NOx with NH3 to N-2 over a Highly Efficient Bifunctional V-alpha-MnOx Catalyst at Low Temperature

Ying Xin, Hao Li, Nana Zhang, Qian Li, Zhaoliang Zhang*, Xiaoming Cao, P. Hu, Lirong Zheng, James A. Anderson

*Corresponding author for this work

Research output: Contribution to journalArticle

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Abstract

Selective catalytic reduction of NOx with ammonia (SCR) is not only an important model catalytic reaction but is also significant in terms of improving environmental air quality and human health. However, SCR catalysts suffer from low activity and selectivity to N-2 at low temperature, which in part may be attributed to our limited understanding of the reaction mechanism. Here, an unambiguous molecular-level mechanism is presented for an improved low-temperature SCR activity using bifunctional catalysts composed of highly active oxides (Mn2O3) for NH3 activation and highly selective vanadates (Mn2V2O7) that promote N-2 formation. NH3 is initially activated by Mn2O3 to form an NH2 intermediate. Transfer of NH2 to Mn2V2P7 then takes place, which facilitates the capture of gaseous NO leading to the formation of NH2NO over Mn2V2O7, whereafter NH2NO is efficiently converted to the preferred N-2 rather than the undesired byproduct, N2O. The proximity of the two components achieved via sol gel preparation plays a crucial role in the transfer of active intermediates.

Original languageEnglish
Pages (from-to)4937-4949
Number of pages25
JournalACS Catalysis
Volume8
Issue number6
Early online date23 Apr 2018
DOIs
Publication statusPublished - Jun 2018

Keywords

  • nitrogen oxides
  • selective catalytic reduction
  • bifunctional catalyst
  • density functional theory
  • mechanism
  • MANGANESE OXIDE CATALYSTS
  • TOTAL-ENERGY CALCULATIONS
  • TI AMORPHOUS OXIDES
  • WAVE BASIS-SET
  • ACTIVE-SITES
  • HYBRID CATALYSTS
  • NITRIC-OXIDE
  • MNOX-CEO2 CATALYST
  • REACTION-MECHANISM
  • SUPERIOR CATALYST

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