NO x and Hydrocarbon Trapping and Conversion in a Sequential Three-Zone Monolith: Spatiotemporal Features

Gupta, Abhay; Ambast, Mugdha; Harold, Michael P.

doi:10.1021/acsengineeringau.2c00023

Title: NO _x and Hydrocarbon Trapping and Conversion in a Sequential Three-Zone Monolith: Spatiotemporal Features

Journal Article · Fri Jul 08 00:00:00 EDT 2022 · ACS Engineering Au

DOI:https://doi.org/10.1021/acsengineeringau.2c00023· OSTI ID:1875603

Gupta, Abhay ^[1]; Ambast, Mugdha ^[1];

^[1]

Department of Chemical & Biomolecular Engineering, University of Houston, Houston, Texas 77204, United States

The spatiotemporal features of the multifunctional monolithic lean hydrocarbon NO_x trap (LHCNT), for eliminating NO_x (x = 1 and 2) and ethylene (C₂H₄), are examined using spatially resolved mass spectrometry (SpaciMS), spanning the sequentially positioned passive NO_x adsorber (PNA; Pd/SSZ-13), hydrocarbon trap (HCT; Pd/BEA), and oxidation catalyst (OC; Pt/Al₂O₃–CeO₂). The overall LHCNT performance is captured in temporal trapping efficiency profiles, which show the integral NO and C₂H₄ uptake followed by delayed NO release along with NO and ethylene oxidation. Spatially resolved transient concentration profiles spanning uptake, release, and conversion of NO, H₂, and C₂H₄, alone or as mixtures in feeds containing H₂O, provide detailed insight into the transient coupling not attainable with effluent concentration monitoring alone. The PNA serves as the primary zone for NO uptake, followed by the OC and HCT. NO oxidation to NO₂ occurs during NO uptake in the PNA due to Pd(II) reduction, while more extensive oxidation occurs in the OC at higher temperature. C₂H₄ uptake and oxidation occur in each of the functions with oxidation occurring the earliest (lowest temperature) in the OC. NO uptake in the PNA and HCT is negligibly affected by H₂ but protracted oxidation of H₂ during the temperature ramp delays NO release, suggesting persistence of NO bound on Pd(I). Both the PNA and HCT exhibit excellent C₂H₄ uptake, which diminishes in the presence of NO. Spatially resolved concentration data reveal several interesting features, such as high-temperature, sequential NO oxidation (by O₂ to NO₂) and C₂H₄ oxidation (by NO₂ to NO + CO₂) in the PNA. Simulated warmup experiments reveal that the LHCNT NO trapping is enhanced with C₂H₄ addition but that a reduction in space velocity may be needed to improve performance. A previously developed PNA model predicts satisfactorily the main features of spatially resolved NO and NO + C₂H₄ data.

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Research Organization:: Univ. of Houston, TX (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: EE0008233

OSTI ID:: 1875603

Alternate ID(s):: OSTI ID: 1906790

Journal Information:: ACS Engineering Au, Journal Name: ACS Engineering Au Vol. 2 Journal Issue: 6; ISSN 2694-2488

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Passive NOx adsorption on Pd/H-ZSM-5: Experiments and modeling Ambast, Mugdha; Karinshak, Kyle; Rahman, Bhuiyan Md. Mushfikur Applied Catalysis B: Environmental, Vol. 269 https://doi.org/10.1016/j.apcatb.2020.118802	journal	July 2020
The first non-precious metal passive NOx adsorber for cold-start applications Jiang, Qiuren; Wang, Chen; Shen, Meiqing Catalysis Communications, Vol. 125 https://doi.org/10.1016/j.catcom.2019.04.004	journal	May 2019
Steady-state and dynamic hysteresis effects during lean co-oxidation of CO and C3H6 over Pt/Al2O3 monolithic catalyst Raj, Richa; Harold, Michael P.; Balakotaiah, Vemuri Chemical Engineering Journal, Vol. 281 https://doi.org/10.1016/j.cej.2015.06.057	journal	December 2015
Passive NO Adsorption on Hydrothermally Aged Pd-Based Small-Pore Zeolites Shan, Yulong; Sun, Yu; Li, Yaobin Topics in Catalysis, Vol. 63, Issue 9-10 https://doi.org/10.1007/s11244-020-01352-6	journal	August 2020
Catalytic Reduction of Nitric Oxide with Ammonia over Transition Metal Ion-Exchanged y Zeolites Seiyama, Tetsuro; Arakawa, Tsuyoshi; Matsuda, Toshio Chemistry Letters, Vol. 4, Issue 7 https://doi.org/10.1246/cl.1975.781	journal	July 1975
Assessing intrusion by the capillary during spatially resolved mass spectrometry measurement Nguyen, Hoang; Peng, Po Yu; Luss, Dan Chemical Engineering Journal, Vol. 307 https://doi.org/10.1016/j.cej.2016.08.101	journal	January 2017
A study of steam reforming of hydrocarbon fuels on Pd/ceria Wang, X.; Gorte, R. J. Applied Catalysis A: General, Vol. 224, Issue 1-2 https://doi.org/10.1016/S0926-860X(01)00783-9	journal	January 2002
Sustained concentration and temperature oscillations in a diesel oxidation catalyst Peng, Po-Yu; Harold, Michael P.; Luss, Dan Chemical Engineering Journal, Vol. 336 https://doi.org/10.1016/j.cej.2017.12.023	journal	March 2018
SpaciMS: spatial and temporal operando resolution of reactions within catalytic monoliths Sá, Jacinto; Fernandes, Daniel Luis Abreu; Aiouache, Farid The Analyst, Vol. 135, Issue 9 https://doi.org/10.1039/c0an00303d	journal	January 2010
Catalytic and ESR studies of ethylene dimerization on palladium-exchanged NaX and CaX zeolites Ghosh, Ashim K.; Kevan, Larry The Journal of Physical Chemistry, Vol. 92, Issue 15 https://doi.org/10.1021/j100326a039	journal	July 1988
Experimental and Theoretical Evidence for the Promotional Effect of Acid Sites on the Diffusion of Alkenes through Small‐Pore Zeolites Cnudde, Pieter; Redekop, Evgeniy A.; Dai, Weili Angewandte Chemie, Vol. 133, Issue 18 https://doi.org/10.1002/ange.202017025	journal	March 2021
Kinetics and multiple rate states of CO oxidation on Pt I. Model development and multiplicity analysis Harold, M. Journal of Catalysis, Vol. 127, Issue 2 https://doi.org/10.1016/0021-9517(91)90182-4	journal	February 1991
Comparison of Pt-BaO/Al2O3 and Pt-CeO2/Al2O3 for NOx storage and reduction: Impact of cycling frequency Zhou, Zhiyu; Harold, Michael P.; Luss, Dan Applied Catalysis B: Environmental, Vol. 255 https://doi.org/10.1016/j.apcatb.2019.05.044	journal	October 2019
The Role of Nickel and Brønsted Sites on Ethylene Oligomerization with Ni-H-Beta Catalysts Seufitelli, Gabriel V. S.; Park, Jason J. W.; Tran, Phuong N. Catalysts, Vol. 12, Issue 5 https://doi.org/10.3390/catal12050565	journal	May 2022
Unravelling the mechanism of NO and NO2 storage in ceria: The role of defects and Ce-O surface sites Filtschew, Anastasia; Hess, Christian Applied Catalysis B: Environmental, Vol. 237 https://doi.org/10.1016/j.apcatb.2018.06.058	journal	December 2018

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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