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Kwak, Ja Hun
Molecular Catalysis lab
Research Interests
  • Heterogeneous catalysis, molecular catalysis, ASlumima, zeolites

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Structure-activity relationships in NH3-SCR over Cu-SSZ-13 as probed by reaction kinetics and EPR studies

Cited 38 times inthomson ciCited 21 times inthomson ci
Title
Structure-activity relationships in NH3-SCR over Cu-SSZ-13 as probed by reaction kinetics and EPR studies
Author
Gao, FengWalter, Eric D.Karp, Eric M.Luo, JinyongTonkyn, Russell G.Kwak, JahunSzanyi, JanosPeden, Charles H. F.
Keywords
Cu-SSZ-13; Electron paramagnetic resonance; Mass-transfer limitation; Reaction kinetics; Selective catalytic reduction; Temperature-programmed reduction
Issue Date
201304
Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
Citation
JOURNAL OF CATALYSIS, v.300, no., pp.20 - 29
Abstract
Cu-SSZ-13 catalysts with various Cu loadings were prepared via aqueous solution ion-exchange. The hydrated samples were characterized with Electron Paramagnetic Resonance (EPR). Cu2+ ion coordination numbers were obtained by analyzing the hyperfine structures, while Cu-Cu distances were estimated from line broadening of the EPR features. By examining EPR and temperature-programmed reduction (TPR) results, two Cu2+ ion locations are suggested. Standard NH3-SCR, as well as non-selective NH3 oxidation reaction with O2, were carried out over these catalysts at high-space velocities. For the SCR reaction, intra-particle diffusion limitations are found. The kinetic data allow for reactant diffusivities to be estimated. However, clear structure-activity relationships for the SCR reaction cannot be derived due to this diffusion limitation. The slower NH3 oxidation reaction, on the other hand, is kinetically limited at low temperatures, and, therefore allows for a correlation between Cu2+ ion location and reaction kinetics to be made.
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DOI
http://dx.doi.org/10.1016/j.jcat.2012.12.020
ISSN
0021-9517
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