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Title: Development of Passive HC/NOx Trap Catalysts for Low Temperature Gasoline Applications

Technical Report ·
DOI:https://doi.org/10.2172/1827367· OSTI ID:1827367
 [1];  [1];  [2];  [2];  [3];  [3];  [3];  [1];  [1];  [4];  [4];  [4];  [4];  [4];  [5];  [6]
  1. Univ. of Kentucky, Lexington, KY (United States)
  2. Univ. of California, Berkeley, CA (United States)
  3. Purdue Univ., West Lafayette, IN (United States)
  4. Ford Motor Company, Detroit, MI (United States)
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Fuels, Engines and Emissions Research Center (FEERC)
  6. BASF Corporation, Florham Park, NJ (United States)

This project aimed to develop fundamental understanding of the chemistry of NO adsorption and reaction in Pd/zeolites so as to facilitate the rational design of passive NOx adsorber catalysts. The approach adopted combined both experimental and computational methods, which together allow a deeper understanding of the governing chemistry than the use of either method alone. The workflow began with Pd/H-CHA and Pd/H-BEA catalyst synthesis and characterization, in which the Si/Al ratio and Al siting were systematically varied. This was followed by catalyst evaluation using temperature-programed adsorption/desorption methods, as well as in situ spectroscopic measurements to probe the chemistry of NO adsorption. In parallel, the adsorption of NO and other relevant species (H2O, CO, HCs) was studied by means of quantum chemical calculations in order to rationalize the experimental data and provide additional insights. Catalyst aging studies were also performed with the aim of elucidating the mechanism of catalyst degradation. Finally, the insights gained in this project were applied to the preparation of an optimized HC/NOx adsorber catalyst, the performance of which was studied using exhaust gas from an engine dynamometer.

Research Organization:
Univ. of Kentucky, Lexington, KY (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office
DOE Contract Number:
EE0008213
OSTI ID:
1827367
Report Number(s):
DOE-UKY-EE0008213
Resource Relation:
Related Information: 1. J. Van der Mynsbrugge, M. Head-Gordon, A.T. Bell, “Computational Modeling Predicts the Stability of Both Pd+ and Pd2+ Ion-Exchanged into H-CHA”, J Mater. Chem. A 2021, https://doi.org/10.1039/d0ta11254b.2. T.M. Lardinois, J.S. Bates, H.H. Lippie, C.K. Russell, J.T. Miller, H. Meyer III, K.A. Unocic, V. Prikhodko, X. Wei, C.K. Lambert, A.B. Getsoian, R. Gounder, “Structural Interconversion between Agglomerated Palladium Domains and Mononuclear Pd(II) Cations in Chabazite Zeolites”, Chem. Mater. 2021, 33(5), 1698–1713; https://doi.org/10.1021/acs.chemmater.0c044653. J.R. Theis and J.A. Ura, “Assessment of Zeolite-Based Low Temperature NOx Adsorbers: Effect of Reductants During Multiple Sequential Cold Starts”, Catal. Today, 2021, 360, 340-349.4. R. Pace, T.M. Lardinois, Y. Ji, R. Gounder, O. Heintz, M. Crocker, “Effects of treatment conditions on Pd speciation in CHA and Beta zeolites for passive NOx adsorption”, ACS Omega, 2021, https://doi.org/10.1021/acsomega.1c03440.5. H. Aljama, M. Head-Gordon, A.T. Bell, "Assessing the stability of Pd-exchanged sites in zeolites with the aid of a high throughput work flow", Nature Communications, under review, 2021. Preprint: https://doi.org/10.21203/rs.3.rs-396201/v1.
Country of Publication:
United States
Language:
English