Determining the storage, availability and reactivity of NH3 within Cu-Chabazite-based Ammonia Selective Catalytic Reduction systems

Phys Chem Chem Phys. 2014 Jan 28;16(4):1639-50. doi: 10.1039/c3cp54132k.

Abstract

Three different types of NH3 species can be simultaneously present on Cu(2+)-exchanged CHA-type zeolites, commonly used in Ammonia Selective Catalytic Reduction (NH3-SCR) systems. These include ammonium ions (NH4(+)), formed on the Brønsted acid sites, [Cu(NH3)4](2+) complexes, resulting from NH3 coordination with the Cu(2+) Lewis sites, and NH3 adsorbed on extra-framework Al (EFAl) species, in contrast to the only two reacting NH3 species recently reported on Cu-SSZ-13 zeolite. The NH4(+) ions react very slowly in comparison to NH3 coordinated to Cu(2+) ions and are likely to contribute little to the standard NH3-SCR process, with the Brønsted groups acting primarily as NH3 storage sites. The availability/reactivity of NH4(+) ions can be however, notably improved by submitting the zeolite to repeated exchanges with Cu(2+), accompanied by a remarkable enhancement in the low temperature activity. Moreover, the presence of EFAl species could also have a positive influence on the reaction rate of the available NH4(+) ions. These results have important implications for NH3 storage and availability in Cu-Chabazite-based NH3-SCR systems.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Ammonia / chemistry*
  • Catalysis
  • Copper / chemistry*
  • Models, Molecular
  • Organometallic Compounds / chemistry*
  • Oxidation-Reduction
  • Surface Properties
  • Temperature
  • Zeolites / chemistry*

Substances

  • Organometallic Compounds
  • chabazite
  • Zeolites
  • Ammonia
  • Copper