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

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Following the movement of Cu ions in a SSZ-13 zeolite during dehydration, reduction and adsorption: A combined in situ TP-XRD, XANES/DRIFTS study

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Title
Following the movement of Cu ions in a SSZ-13 zeolite during dehydration, reduction and adsorption: A combined in situ TP-XRD, XANES/DRIFTS study
Author
Kwak, JahunVarga, TamásPeden, Charles H.F.Gao, FengHanson, Jonathan C.Szanyi, János
Keywords
Cation coordination; Cation movement; Cu-SSZ-13; DRIFTS; XANES; XRD
Issue Date
201405
Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
Citation
JOURNAL OF CATALYSIS, v.314, no., pp.83 - 93
Abstract
Cu-SSZ-13 has been shown to possess high activity and superior N 2 formation selectivity in the selective catalytic reduction of NOx under oxygen rich conditions. Here, a combination of synchrotron-based (XRD and XANES) and vibrational (DRIFTS) spectroscopy tools has been used to follow the changes in the location and coordination environment of copper ions in a Cu-SSZ-13 zeolite during calcinations, reduction with CO, and adsorption of CO and H2O. XANES spectra collected during these procedures provide critical information not only on the variation in the oxidation state of the copper species in the zeolite structure, but also on the changes in the coordination environment around these ions as they interact with the framework, and with different adsorbates (H2O and CO). Time-resolved XRD data indicate the movement of copper ions and the consequent variation of the unit cell parameters during dehydration. DRIFT spectra provide information about the adsorbed species present in the zeolite, as well as the oxidation states of and coordination environment around the copper ions. A careful analysis of the asymmetric T-O-T vibrations of the CHA framework perturbed by copper ions in different coordination environments proved to be especially informative. The results of this study will aid the identification of the location, coordination and oxidation states of copper ions obtained during in operando catalytic studies
URI
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DOI
http://dx.doi.org/10.1016/j.jcat.2014.03.003
ISSN
0021-9517
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