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NOx Adsorber Materials: Fundamental Studies, and Investigations of Sulfur Poisoning and Thermal Deactivation


EMSL Project ID
35404

Abstract

Catalysits systems related to automotive exhaust control will be investigated. Specifically, the focus will be on catalysts that are important in lean NOx emission control (NOx storage/reduction (NSR)catalysts; catalysts for selective catalyitc reduction (SCR) of NOx). On the NSR side we are going to continue our fundamental studies aimed at understanding the sulfur poisoning of BaO-based catalysts. The effect of CeO2 addition to the base Pt/BaO/Al2O3 catalyst will also be studies, both in the view of NOx uptake/release/reduction and sulfur poisoning. On the SCR side, we are going to study the deactivation mechanisms of zeolite-based SCR catalysts (e.g. dealumination, sulfur poisoning, active phase agglomeration, etc).

Project Details

Project type
Large-Scale EMSL Research
Start Date
2009-10-05
End Date
2012-09-30
Status
Closed

Team

Principal Investigator

Charles Peden
Institution
Pacific Northwest National Laboratory

Team Members

James Lownsbury
Institution
University of Washington

Aleksei Vjunov
Institution
Pacific Northwest National Laboratory

Jin-Yong Luo
Institution
Pacific Northwest National Laboratory

Jong Lee
Institution
Pacific Northwest National Laboratory

Hye Sun Shin
Institution
Chonnam National University

Ik Jun Jang
Institution
Chonnam National University

Feng Gao
Institution
Pacific Northwest National Laboratory

Haiyang Zhu
Institution
Pacific Northwest National Laboratory

Donghai Mei
Institution
Tiangong University

Yisun Cheng
Institution
Ford Motor Company

William Epling
Institution
University of Waterloo

Ja Hun Kwak
Institution
Ulsan National Institute of Science and Technology

Russell Tonkyn
Institution
Pacific Northwest National Laboratory

Janos Szanyi
Institution
Pacific Northwest National Laboratory

Do Heui Kim
Institution
Seoul National University

Diana Tran
Institution
Pacific Northwest National Laboratory

Related Publications

Cheng Y, C Lambert, DH Kim, JH Kwak, SJ Cho, and CHF Peden. 2010. "The Different Impacts of SO2 and SO3 on Cu/Zeolite SCR Catalysts." Catalysis Today 151(3-4):266-270. doi:10.1016/j.cattod.2010.01.013
Jeon JK, H Kim, YK Park, CHF Peden, and DH Kim. 2011. "Regeneration of field-spent activated carbon catalysts for low-temperature selective catalytic reduction of NOx with NH3." Chemical Engineering Journal 174(1):242-248. doi:10.1016/j.cej.2011.09.011
Kim DH, A Yezerets, J Li, N Currier, H Chen, H. Hess, MH Engelhard, GG Muntean, and CHF Peden. 2012. "Effect of sulfur loading on the desulfation chemistry of a commercial lean NOx trap catalyst." Catalysis Today. doi:10.1016/j.cattod.2012.05.040
Kim DH, KK Mudiyanselage, J Szanyi, H Zhu, JH Kwak, and CHF Peden. 2012. "Characteristics of Pt-K/MgAl2O4 lean NOx trap catalysts." Catalysis Today 184(1):2-7. doi:10.1016/j.cattod.2011.11.024
Kim, D.H.; Kwak, J.H.; Szanyi, J.; Wang, X.; Li, G.; Hanson, J.C.; Peden, C.H.F. "Characteristics of Desulfation Behavior for Presulfated Pt-BaO/CeO2 Lean NOx Trap Catalysts: The Role of the CeO2 Support." J. Phys. Chem. C 113 (2009) 21123-21129.
Kim, D.H.; Kwak, J.H.; Szanyi, J.; Wang, X.; Peden, C.H.F. 2009. "Promotional effects of CO2 on Desulfation Processes for Pre-Sulfated Pt-BaO/Al2O3 Lean NOx Trap Catalysts." Topics in Catal. 52(13-20):1719-1722. DOI 10.1007/s11244-009-9328-8
Kim, D.H.; Szanyi, J.; Kwak, J.H.; Wang, X.; Hanson, J.C.; Engelhard, M.; Peden, C.H.F. 2009. "Effects of Sulfation Level on the Desulfation Behavior of Pre-Sulfated Pt-BaO/Al2O3 Lean NOx Trap Catalysts: A Combined H2 TPRX, In-Situ Sulfur K-Edge XANES, XPS and TR-XRD Study." J. Phys. Chem. C 113(17):7336-7341. DOI: 10.1021/jp900304h
Kwak JH, DH Kim, J Szanyi, SJ Cho, and CHF Peden. 2012. "Enhanced high temperature performance of MgAl2O4-supported Pt-BaO lean NOx trap catalysts." Topics in Catalysis 55(1-2):70-77. doi:10.1007/s11244-012-9779-1
Kwak JH, DN Tran, J Szanyi, CHF Peden, and JH Lee. 2012. "The Effect of Copper Loading on the Selective Catalytic Reduction of Nitric Oxide by Ammonia Over Cu-SSZ-13." Catalysis Letters 142(3):295-301. doi:10.1007/s10562-012-0771-y
Kwak JH, DN Tran, SD Burton, J Szanyi, JH Lee, and CHF Peden. 2012. "Effects of Hydrothermal Aging on NH3-SCR reaction over Cu/zeolites." Journal of Catalysis 287(1):203-209. doi:10.1016/j.jcat.2011.12.025
Kwak, J.H.; Hu, J.; Mei, D.; Yi, C.-W.; Kim, D.H.; Peden, C.H.F.; Allard, L.; Szanyi, J. 2009. "Coordinatively Unsaturated Al+3 Centers as Binding Sites for Active Catalyst Phases: Strong Interactions Between Pt and gamma-Al2O3 Surfaces." Science 325(5948):1670-1673. DOI: 10.1126/science.1176745
Kwak JH, H Zhu, JH Lee, CHF Peden, and J Szanyi. 2012. "Two different cationic positions in Cu-SSZ-13? ." Chemical Communications 48(39):4758-4760. doi:10.1039/C2CC31184D
Kwak, J.H.; Mei, D.; Yi, C.-W.; Kim, D.H.; Peden, C.H.F.; Allard, L.F.; Szanyi, J. 2009. "Understanding the Nature of Surface Nitrates in BaO/gamma-Al2O3 NOx Storage Materials: A Combined Experimental and Theoretical Study." J. Catal. 261(1):17-22.
Kwak JH, RG Tonkyn, DH Kim, J Szanyi, and CHF Peden. 2010. "Excellent activity and selectivity of Cu-SSZ-13 in the selective catalytic reduction of NOx with NH3." Journal of Catalysis 275(2):187-190. doi:10.1016/j.jcat.2010.07.031
Luo J, F Gao, DH Kim, and CHF Peden. 2014. "Effects of Potassium loading and thermal aging on K/Pt/Al2O3 high-temperature lean NOx trap catalysts." Catalysis Today. doi:10.1016/j.cattod.2013.12.020
Mei, D.; Ge, Q.; Kwak, J.H.; Kim, D.H.; Verrier, C.; Szanyi, J.; Peden, C.H.F. 2009. "Characterization of Surface and Bulk Nitrates of gamma-Al2O3-Supported Alkaline Earth Oxides using Density Functional Theory." Phys. Chem. Chem. Phys. 11 (2009) 3380-3389.
Mei, D.; Ge, Q.; Szanyi, J.; Peden, C.H.F. 2009. "A First-Principles Analysis of NOx Adsorption on Anhydrous gamma-Al2O3 Surfaces." J. Phys. Chem. C 113(18):7779-7789. DOI: 10.1021/jp8103563
Mei D, JH Kwak, J Szanyi, Q Ge, and CHF Peden. 2010. "Catalyst Size and Morphological Effects on the Interaction of NO2 with BaO/?-Al2O3 Materials ." Catalysis Today 151(3-4):304-313. doi:10.1016/j.cattod.2010.01.005
Mei D, JH Kwak, JZ Hu, SJ Cho, J Szanyi, L Allard, and CHF Peden. 2010. "The Unique Role of Anchoring Penta-coordinated Al3+ Sites in the Sintering of ? Al2O3-supported Pt Catalysts ." The Journal of Physical Chemistry Letters 1(18):2688–2691. doi:10.1021/jz101073p
Peden CHF, JH Kwak, SD Burton, RG Tonkyn, DH Kim, JH Lee, HW Jen, G Cavattaio, Y Cheng, and C Lambert. 2012. "Possible Origin of Improved High Temperature Performance of Hydrothermally Aged Cu/Beta Zeolite Catalysts." Catalysis Today 184(1):245-251. doi:10.1016/j.cattod.2011.11.008
Schmieg SJ, SH Oh, CH Kim, DB Brown, JH Lee, CHF Peden, and DH Kim. 2012. "Thermal Durability of Cu-CHA NH3-SCR Catalysts for Diesel NOx Reduction." Catalysis Today 184(1):252-261. doi:10.1016/j.cattod.2011.10.034
She, X.; Flytzani-Stephanopoulos, M.; Wang., C.; Wang, Y.; Peden, C.H.F. 2009. "SO2-induced stability of Ag-alumina catalysts in the SCR of NO with methane." Appl. Catal. B 88(1-2):98-105.
Szanyi J, JH Kwak, H Zhu, and CHF Peden. 2013. "Characterization of Cu-SSZ-13 NH3 SCR Catalysts: an in situ FTIR Study." Physical Chemistry Chemical Physics. PCCP 15(7):2368-2380. doi:10.1039/c2cp43467a
Wang X, DH Kim, JH Kwak, CM Wang, J Szanyi, and CHF Peden. 2011. "Effect of reductive treatments on Pt behavior and NOx storage in lean NOx trap catalysts." Catalysis Today 175(1):78– 82. doi:10.1016/j.cattod.2011.03.032
Wang X, JC Hanson, JH Kwak, J Szanyi, and CHF Peden. 2013. "Cation Movements during Dehydration and NO2 Desorption in a Ba-Y,FAU zeolite: an in situ Time-resolved X-ray Diffraction Study." Journal of Physical Chemistry C 117(8):3915-3922. doi:10.1021/jp308307m
Wiebenga MH, CH Kim, SJ Schmieg, SH Oh, DB Brown, DH Kim, JH Lee, and CHF Peden. 2012. "Deactivation Mechanisms of Pt/Pd-based Diesel Oxidation Catalysts." Catalysis Today 184(1):197-204. doi:10.1016/j.cattod.2011.11.014
Yezerets A, CHF Peden, J Szanyi, I Nova, and B Epling. 2012. "Preface: Special Issue on Catalytic Control of Lean-Burn Engine Exhaust Emissions." Catalysis Today 184(1):1. doi:10.1016/j.cattod.2012.02.011