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Title: Effects of Hydrothermal Aging on NH3-SCR reaction over Cu/zeolites

Abstract

The effects of hydrothermal treatment on model Cu/zeolite catalysts were investigated to better understand the nature of Cu species for the selective catalytic reduction of NO{sub x} by NH{sub 3}. After hydrothermal aging at 800 C for 16 h, the NO{sub x} reduction performance of Cu-ZSM-5 and Cu-beta were significantly reduced at low temperatures, while that of Cu-SSZ-13 was not affected. When the zeolite framework aluminum species were probed using solid state {sup 27}Al-NMR, significant reduction in the intensities of the tetrahedral aluminum peak was observed for Cu-ZSM-5 and Cu-beta, although no increase in the intensities of the octahedral aluminum peak was observed. When the redox behavior of Cu species was examined using H{sub 2}-TPR, it was found that Cu{sup 2+} could be reduced to Cu{sup +} and to Cu{sup 0} fir Cu-ZSM-5 and Cu-beta catalysts, while Cu{sup 2+} could be reduced to Cu{sup +} only for Cu-SSZ-13. After hydrothermal aging, CuO and Cu-aluminate species were found to form in Cu-ZSM-5 and Cu-beta, while little changes were observed for Cu-SSZ-13.

Authors:
; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1034968
Report Number(s):
PNNL-SA-81754
Journal ID: ISSN 0021-9517; JCTLA5; 35404; VT0401000; TRN: US201204%%261
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Journal of Catalysis
Additional Journal Information:
Journal Volume: 287; Journal Issue: 1; Journal ID: ISSN 0021-9517
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; AGING; ALUMINIUM; CATALYSTS; COPPER; PERFORMANCE; SELECTIVE CATALYTIC REDUCTION; TEMPERATURE DEPENDENCE; ZEOLITES; Environmental Molecular Sciences Laboratory

Citation Formats

Kwak, Ja Hun, Tran, Diana N, Burton, Sarah D, Szanyi, Janos, Lee, Jong H, and Peden, Charles HF. Effects of Hydrothermal Aging on NH3-SCR reaction over Cu/zeolites. United States: N. p., 2012. Web. doi:10.1016/j.jcat.2011.12.025.
Kwak, Ja Hun, Tran, Diana N, Burton, Sarah D, Szanyi, Janos, Lee, Jong H, & Peden, Charles HF. Effects of Hydrothermal Aging on NH3-SCR reaction over Cu/zeolites. United States. https://doi.org/10.1016/j.jcat.2011.12.025
Kwak, Ja Hun, Tran, Diana N, Burton, Sarah D, Szanyi, Janos, Lee, Jong H, and Peden, Charles HF. 2012. "Effects of Hydrothermal Aging on NH3-SCR reaction over Cu/zeolites". United States. https://doi.org/10.1016/j.jcat.2011.12.025.
@article{osti_1034968,
title = {Effects of Hydrothermal Aging on NH3-SCR reaction over Cu/zeolites},
author = {Kwak, Ja Hun and Tran, Diana N and Burton, Sarah D and Szanyi, Janos and Lee, Jong H and Peden, Charles HF},
abstractNote = {The effects of hydrothermal treatment on model Cu/zeolite catalysts were investigated to better understand the nature of Cu species for the selective catalytic reduction of NO{sub x} by NH{sub 3}. After hydrothermal aging at 800 C for 16 h, the NO{sub x} reduction performance of Cu-ZSM-5 and Cu-beta were significantly reduced at low temperatures, while that of Cu-SSZ-13 was not affected. When the zeolite framework aluminum species were probed using solid state {sup 27}Al-NMR, significant reduction in the intensities of the tetrahedral aluminum peak was observed for Cu-ZSM-5 and Cu-beta, although no increase in the intensities of the octahedral aluminum peak was observed. When the redox behavior of Cu species was examined using H{sub 2}-TPR, it was found that Cu{sup 2+} could be reduced to Cu{sup +} and to Cu{sup 0} fir Cu-ZSM-5 and Cu-beta catalysts, while Cu{sup 2+} could be reduced to Cu{sup +} only for Cu-SSZ-13. After hydrothermal aging, CuO and Cu-aluminate species were found to form in Cu-ZSM-5 and Cu-beta, while little changes were observed for Cu-SSZ-13.},
doi = {10.1016/j.jcat.2011.12.025},
url = {https://www.osti.gov/biblio/1034968}, journal = {Journal of Catalysis},
issn = {0021-9517},
number = 1,
volume = 287,
place = {United States},
year = {Mon Feb 06 00:00:00 EST 2012},
month = {Mon Feb 06 00:00:00 EST 2012}
}