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

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HPC-UGent: the central High Performance Computing infrastructure of Ghent University
Abstract
Three different types of NH3 species can be simultaneously present on Cu2+-exchanged CHA-type zeolites, commonly used in Ammonia Selective Catalytic Reduction (NH3-SCR) systems. These include ammonium ions (NH4+), formed on the Bronsted acid sites, [Cu(NH3)(4)](2+) complexes, resulting from NH3 coordination with the Cu2+ 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 Cu2+ ions and are likely to contribute little to the standard NH3-SCR process, with the Bronsted 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 Cu2+, 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.
Keywords
SCR CATALYSTS, EXCHANGED SSZ-13, FE-ZSM-5 CATALYST, NANOCRYSTALLINE NAY, ALUMINUM DISTRIBUTION, ACTIVE-SITES, NITRIC-OXIDE, MOLECULAR-DYNAMICS, NOX REDUCTION, BETA-ZEOLITE

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Citation

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MLA
Lezcano-Gonzalez, Ines, Upakul Deka, Bjørnar Arstad, et al. “Determining the Storage, Availability and Reactivity of NH3 Within Cu-Chabazite-based Ammonia Selective Catalytic Reduction Systems.” PHYSICAL CHEMISTRY CHEMICAL PHYSICS 16.4 (2014): 1639–1650. Print.
APA
Lezcano-Gonzalez, I., Deka, U., Arstad, B., Van Yperen-De Deyne, A., Hemelsoet, K., Waroquier, M., Van Speybroeck, V., et al. (2014). Determining the storage, availability and reactivity of NH3 within Cu-Chabazite-based Ammonia Selective Catalytic Reduction systems. PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 16(4), 1639–1650.
Chicago author-date
Lezcano-Gonzalez, Ines, Upakul Deka, Bjørnar Arstad, Andy Van Yperen-De Deyne, Karen Hemelsoet, Michel Waroquier, Veronique Van Speybroeck, Bert M Weckhuysen, and Andrew M Beale. 2014. “Determining the Storage, Availability and Reactivity of NH3 Within Cu-Chabazite-based Ammonia Selective Catalytic Reduction Systems.” Physical Chemistry Chemical Physics 16 (4): 1639–1650.
Chicago author-date (all authors)
Lezcano-Gonzalez, Ines, Upakul Deka, Bjørnar Arstad, Andy Van Yperen-De Deyne, Karen Hemelsoet, Michel Waroquier, Veronique Van Speybroeck, Bert M Weckhuysen, and Andrew M Beale. 2014. “Determining the Storage, Availability and Reactivity of NH3 Within Cu-Chabazite-based Ammonia Selective Catalytic Reduction Systems.” Physical Chemistry Chemical Physics 16 (4): 1639–1650.
Vancouver
1.
Lezcano-Gonzalez I, Deka U, Arstad B, Van Yperen-De Deyne A, Hemelsoet K, Waroquier M, et al. Determining the storage, availability and reactivity of NH3 within Cu-Chabazite-based Ammonia Selective Catalytic Reduction systems. PHYSICAL CHEMISTRY CHEMICAL PHYSICS. 2014;16(4):1639–50.
IEEE
[1]
I. Lezcano-Gonzalez et al., “Determining the storage, availability and reactivity of NH3 within Cu-Chabazite-based Ammonia Selective Catalytic Reduction systems,” PHYSICAL CHEMISTRY CHEMICAL PHYSICS, vol. 16, no. 4, pp. 1639–1650, 2014.
@article{4246850,
  abstract     = {Three different types of NH3 species can be simultaneously present on Cu2+-exchanged CHA-type zeolites, commonly used in Ammonia Selective Catalytic Reduction (NH3-SCR) systems. These include ammonium ions (NH4+), formed on the Bronsted acid sites, [Cu(NH3)(4)](2+) complexes, resulting from NH3 coordination with the Cu2+ 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 Cu2+ ions and are likely to contribute little to the standard NH3-SCR process, with the Bronsted 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 Cu2+, 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.},
  author       = {Lezcano-Gonzalez, Ines and Deka, Upakul and Arstad, Bjørnar and Van Yperen-De Deyne, Andy and Hemelsoet, Karen and Waroquier, Michel and Van Speybroeck, Veronique and Weckhuysen, Bert M and Beale, Andrew M},
  issn         = {1463-9076},
  journal      = {PHYSICAL CHEMISTRY CHEMICAL PHYSICS},
  keywords     = {SCR CATALYSTS,EXCHANGED SSZ-13,FE-ZSM-5 CATALYST,NANOCRYSTALLINE NAY,ALUMINUM DISTRIBUTION,ACTIVE-SITES,NITRIC-OXIDE,MOLECULAR-DYNAMICS,NOX REDUCTION,BETA-ZEOLITE},
  language     = {eng},
  number       = {4},
  pages        = {1639--1650},
  title        = {Determining the storage, availability and reactivity of NH3 within Cu-Chabazite-based Ammonia Selective Catalytic Reduction systems},
  url          = {http://dx.doi.org/10.1039/c3cp54132k},
  volume       = {16},
  year         = {2014},
}

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