文献类型：期刊文献

英文题名：Catalytic N2O decomposition and reduction by NH3 over Fe/Beta and Fe/SSZ-13 catalysts

作者：Wang, Aiyong[1,2];Wang, Yilin[2];Walter, Eric D.[3];Kukkadapu, Ravi K.[3];Guo, Yanglong[1];Lu, Guanzhong[1];Weber, Robert S.[2];Wang, Yong[2];Peden, Charles H. F.[2];Gao, Feng[2]

机构：[1]East China Univ Sci & Technol, Res Inst Ind Catalysis, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[2]Pacific Northwest Natl Lab, Inst Integrated Catalysis, POB 999, Richland, WA 99352 USA;[3]Pacific Northwest Natl Lab, Environm Mol Sci Lab, POB 999, Richland, WA 99352 USA

年份：2018

卷号：358

起止页码：199

外文期刊名：JOURNAL OF CATALYSIS

收录：;EI(收录号：20180204621257);WOS:【SCI-EXPANDED(收录号:WOS:000424718900021)】；

基金：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 a Joint-Training Scholarship Program with PNNL. The authors from East China University of Science and Technology acknowledge the 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 support.

语种：英文

外文关键词：Fe/Beta; Fe/SSZ-13; N2O decomposition; N2O reduction by NH3; Fe active center

摘要：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 materials were synthesized via solution ion exchange and used to catalyze these two reactions. The nature of the Fe species was probed with UV-vis, Mossbauer and EPR spectroscopies and H-2-TPR. These characterizations collectively indicate that primarily isolated and dinuclear Fe sites are present in Fe/SSZ-13, whereas Fe/Beta contains higher concentrations of oligomeric FexOy species. H-2-TPR results suggest that Fe-O interactions are weaker in Fe/SSZ-13, as evidenced by the lower reduction temperatures by H-2 and higher extents of autoreduction during high-temperature pretreatments in inert gas. Kinetic measurements show that Fe/SSZ-13 has higher normalized reaction rates in catalytic N2O decomposition, thus demonstrating a positive correlation between reaction rate and Fe-O binding, consistent with O-2 desorption being rate-limiting for this reaction. However, Fe/Beta was found to display higher reaction rates in catalyzing N2O reduction by NH3. This latter result indicates that larger active ensembles (i.e., oligomers) are responsible for this reaction, consistent with the fact that both N2O and NH3 need to be activated in this case. (C) 2017 Elsevier Inc. All rights reserved.