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Title: Catalytic N 2O decomposition and reduction by NH 3 over Fe/Beta and Fe/SSZ-13 catalysts

Abstract

Fe/zeolites are important N 2O abatement catalysts, efficient in direct N 2O decomposition and (selective) catalytic N 2O reduction. In this study, Fe/Beta and Fe/SSZ-13 were synthesized via solution ion-exchange and used to catalyze these two reactions. Nature of the Fe species was probed with UV-vis, Mössbauer and EPR spectroscopies and H2-TPR. The characterizations collectively indicate that isolated and dinuclear Fe sites dominate in Fe/SSZ-13, whereas Fe/Beta contains higher concentrations of oligomeric Fe xO y species. H 2-TPR results suggest that Fe-O interactions are weaker in Fe/SSZ-13, as evidenced by the lower reduction temperatures and higher extents of autoreduction during high-temperature pretreatments in inert gas. Kinetic measurements show that Fe/SSZ-13 has higher activity in catalytic N 2O decomposition, thus demonstrating a positive correlation between activity and Fe-O binding, consistent with O 2 desorption being rate-limiting for this reaction. However, Fe/Beta was found to be more active in catalyzing N 2O reduction by NH 3. This indicates that larger active ensembles (i.e., oligomers) are more active for this reaction, consistent with the fact that both N 2O and NH 3 need to be activated in this case. The authors from PNNL gratefully acknowledge the US Department of Energy (DOE), Energy Efficiencymore » and Renewable Energy, Vehicle Technologies Office for the support of this work. The research described in this paper was performed in the Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by the DOE’s Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory (PNNL). PNNL is operated for the US DOE by Battelle. Aiyong Wang gratefully acknowledges the China Scholarship Council for the Joint-Training Scholarship Program with the Pacific Northwest National Laboratory (PNNL). The authors from East China University of Science and Technology acknowledge National Basic Research Program of China (2013CB933200), National Natural Science Foundation of China (21577035, 21577034), Commission of Science and Technology of Shanghai Municipality (15DZ1205305) and 111 Project (B08021) for supports.« less

Authors:
; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1423414
Report Number(s):
PNNL-SA-128426
Journal ID: ISSN 0021-9517; 47953; VT0401000
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Catalysis; Journal Volume: 358; Journal Issue: C
Country of Publication:
United States
Language:
English
Subject:
Environmental Molecular Sciences Laboratory

Citation Formats

Wang, Aiyong, Wang, Yilin, Walter, Eric D., Kukkadapu, Ravi K., Guo, Yanglong, Lu, Guanzhong, Weber, Robert S., Wang, Yong, Peden, Charles H. F., and Gao, Feng. Catalytic N2O decomposition and reduction by NH3 over Fe/Beta and Fe/SSZ-13 catalysts. United States: N. p., 2018. Web. doi:10.1016/j.jcat.2017.12.011.
Wang, Aiyong, Wang, Yilin, Walter, Eric D., Kukkadapu, Ravi K., Guo, Yanglong, Lu, Guanzhong, Weber, Robert S., Wang, Yong, Peden, Charles H. F., & Gao, Feng. Catalytic N2O decomposition and reduction by NH3 over Fe/Beta and Fe/SSZ-13 catalysts. United States. doi:10.1016/j.jcat.2017.12.011.
Wang, Aiyong, Wang, Yilin, Walter, Eric D., Kukkadapu, Ravi K., Guo, Yanglong, Lu, Guanzhong, Weber, Robert S., Wang, Yong, Peden, Charles H. F., and Gao, Feng. Thu . "Catalytic N2O decomposition and reduction by NH3 over Fe/Beta and Fe/SSZ-13 catalysts". United States. doi:10.1016/j.jcat.2017.12.011.
@article{osti_1423414,
title = {Catalytic N2O decomposition and reduction by NH3 over Fe/Beta and Fe/SSZ-13 catalysts},
author = {Wang, Aiyong and Wang, Yilin and Walter, Eric D. and Kukkadapu, Ravi K. and Guo, Yanglong and Lu, Guanzhong and Weber, Robert S. and Wang, Yong and Peden, Charles H. F. and Gao, Feng},
abstractNote = {Fe/zeolites are important N2O abatement catalysts, efficient in direct N2O decomposition and (selective) catalytic N2O reduction. In this study, Fe/Beta and Fe/SSZ-13 were synthesized via solution ion-exchange and used to catalyze these two reactions. Nature of the Fe species was probed with UV-vis, Mössbauer and EPR spectroscopies and H2-TPR. The characterizations collectively indicate that isolated and dinuclear Fe sites dominate in Fe/SSZ-13, whereas Fe/Beta contains higher concentrations of oligomeric FexOy species. H2-TPR results suggest that Fe-O interactions are weaker in Fe/SSZ-13, as evidenced by the lower reduction temperatures and higher extents of autoreduction during high-temperature pretreatments in inert gas. Kinetic measurements show that Fe/SSZ-13 has higher activity in catalytic N2O decomposition, thus demonstrating a positive correlation between activity and Fe-O binding, consistent with O2 desorption being rate-limiting for this reaction. However, Fe/Beta was found to be more active in catalyzing N2O reduction by NH3. This indicates that larger active ensembles (i.e., oligomers) are more active for this reaction, consistent with the fact that both N2O and NH3 need to be activated in this case. The authors from PNNL gratefully acknowledge the US Department of Energy (DOE), Energy Efficiency and Renewable Energy, Vehicle Technologies Office for the support of this work. The research described in this paper was performed in the Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by the DOE’s Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory (PNNL). PNNL is operated for the US DOE by Battelle. Aiyong Wang gratefully acknowledges the China Scholarship Council for the Joint-Training Scholarship Program with the Pacific Northwest National Laboratory (PNNL). The authors from East China University of Science and Technology acknowledge National Basic Research Program of China (2013CB933200), National Natural Science Foundation of China (21577035, 21577034), Commission of Science and Technology of Shanghai Municipality (15DZ1205305) and 111 Project (B08021) for supports.},
doi = {10.1016/j.jcat.2017.12.011},
journal = {Journal of Catalysis},
number = C,
volume = 358,
place = {United States},
year = {Thu Feb 01 00:00:00 EST 2018},
month = {Thu Feb 01 00:00:00 EST 2018}
}