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Title: Enhanced NO, CO and C3H6 conversion on Pt/Pd catalysts: Impact of oxygen storage material and catalyst architecture

Journal Article · · Catalysis Today
 [1]; ORCiD logo [2];  [2]
  1. Univ. of Houston, TX (United States). Dept. of Chemical and Biomolecular Engineering; Univ. of Houston, TX (United States)
  2. Univ. of Houston, TX (United States). Dept. of Chemical and Biomolecular Engineering

Simultaneous conversion of NO, CO and C3H6 under stoichiometric conditions was carried out on washcoated monoliths containing oxygen storage material (OSM)-promoted mixed Platinum group metals (PGM: Pt(95 %)/Pd(5 %)), to evaluate OSM promotion and to identify the best architecture. The studied OSMs include ceria-zirconia (Ce0.3Zr0.7O2; CZO) and mixed metal oxide spinel (Mn0.5Fe2.5O4; MFO). PGM supported directly on the OSM was found to be the best design for CZO, leading to a ~70 °C simultaneous decrease in the light-off temperature (T80; feed temperature giving 80 % conversion) for NO, CO and C3H6 conversion compared to the alumina-supported PGM. Close coupling between the PGM and CZO is responsible for the activity promotion. In contrast, a dual-layer architecture (top PGM layer, bottom MFO layer) outperformed the MFO-supported PGM catalyst. The dual-layer PGM-MFO catalyst decreased the T80 by ~50 °C for NO, CO and C3H6 conversion compared to the PGM-only catalyst. Enhancement obtained with the dual-layer PGM-MFO architecture relies on a direct catalytic contribution from the spinel. During lean/rich modulation the addition of CZO or spinel helps to mitigate the detrimental impact of modulation on NO, CO and C3H6 conversion above 400 °C. The data suggest that both CZO and MFO can buffer lean/rich modulation but exhibit preference to different reductants; CZO-supported PGM and dual-layer PGM-MFO show no conversion decrease during modulation for CO or C3H6 modulation, respectively. Dynamic oxygen storage capacity (DOSC) measurements show that the spinel exhibits ~10 times higher DOSC than CZO for both CO and C3H6 reductants. Both CO and C3H6 are equally effective reductants for the MFO but CO is better for CZO and PGM-deposited CZO. The study provides useful insight into benefits of OSM and provides guidance for optimization of the multi-component PGM + OSM catalyst composition and architecture.

Research Organization:
Univ. of Houston, TX (United States)
Sponsoring Organization:
USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE)
Grant/Contract Number:
EE0008332
OSTI ID:
1848742
Journal Information:
Catalysis Today, Journal Name: Catalysis Today Journal Issue: C Vol. 360; ISSN 0920-5861
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

References (45)

Oxygen Vacancies in Reduced Rh/ and Pt/Ceria for Highly Selective and Reactive Reduction of NO into N 2 in excess of O 2 journal June 2017
Investigating carbon monoxide and propene oxidation on a platinum diesel oxidation catalyst journal January 2014
Kinetic Study of the CO Oxidation over Pt/γ-Al2O3and Pt/Rh/CeO2/γ-Al2O3in the Presence of H2O and CO2 journal October 1997
The Dynamics of Oxygen Storage in Ceria–Zirconia Model Catalysts Measured by CO Oxidation under Stationary and Cycling Feedstream Compositions journal July 2000
Improved Metal-Support Interaction in Pt/CeO2/SiO2 Catalysts after Zinc Addition journal August 2002
Automotive exhaust catalysis: Is periodic operation beneficial? journal May 1996
Poison-resistant catalysts for the simultaneous control of hydrocarbon, carbon monoxide, and nitrogen oxide emissions*1 journal March 1979
Temperature-programmed reduction. Parametric sensitivity and estimation of kinetic parameters journal October 1983
The oxidation of CO and hydrocarbons over noble metal catalysts journal May 1984
Ceria in automotive exhaust catalysts I. Oxygen storage journal April 1984
Dynamic behavior of three-way catalysts journal June 1986
Periodic operation of catalytic reactors—introduction and overview journal August 1995
Origins of low-temperature three-way activity in Pt/CeO2 journal April 1995
Effect of perturbations in the exhaust gas composition on three-way catalyst light off journal January 2003
Three-way catalytic converter modelling: fast- and slow-oxidizing hydrocarbons, inhibiting species, and steam-reforming reaction journal February 1998
Automotive catalytic converters: current status and some perspectives journal January 2003
Studies of the water-gas-shift reaction on ceria-supported Pt, Pd, and Rh: Implications for oxygen-storage properties journal January 1998
Oxygen storage capacity measurements of three-way catalysts under transient conditions journal January 2002
On the mechanism of fast oxygen storage and release in ceria-zirconia model catalysts journal September 2004
Co-oxidation of CO and propylene on Pd/CeO2-ZrO2 and Pd/Al2O3 monolith catalysts: A light-off, kinetics, and mechanistic study journal December 2017
NOx reduction on Ceria: Impact of lean-rich cycling journal January 2019
Comparison of Pt-BaO/Al2O3 and Pt-CeO2/Al2O3 for NOx storage and reduction: Impact of cycling frequency journal October 2019
Improved activity of Rh/CeO2–ZrO2 three-way catalyst by high-temperature ageing journal January 2010
Oxygen storage capacity and structural properties of Ni-doped LaMnO3 perovskites journal November 2013
Enhanced catalytic activity of ceria nanorods from well-defined reactive crystal planes journal January 2005
Fundamentals and Catalytic Applications of CeO 2 -Based Materials journal April 2016
Perovskites as Geo-inspired Oxygen Storage Materials for Chemical Looping and Three-Way Catalysis: A Perspective journal July 2018
Perovskites as Substitutes of Noble Metals for Heterogeneous Catalysis: Dream or Reality journal September 2014
Behavior of automotive noble metal catalysts in cycled feedstreams
  • Muraki, Hideaki; Shinjoh, Hirofumi; Sobukawa, Hideo
  • Industrial & Engineering Chemistry Product Research and Development, Vol. 24, Issue 1 https://doi.org/10.1021/i300017a009
journal March 1985
Promoting Effect of CeO 2 in Combustion Synthesized Pt/CeO 2 Catalyst for CO Oxidation journal June 2003
Shape-Selective Synthesis and Oxygen Storage Behavior of Ceria Nanopolyhedra, Nanorods, and Nanocubes journal December 2005
Pd-Supported Interaction-Defined Selective Redox Activities in Pd−Ce 0.7 Zr 0.3 O 2 −Al 2 O 3 Model Three-Way Catalysts journal June 2009
Influence of Mutual Platinum-Dispersed Ceria Interactions on the Promoting Effect of Ceria for the CO Oxidation Reaction in a Pt/CeO 2 /Al 2 O 3 Catalyst journal May 1998
A comparative study of oxygen storage capacity over Ce0.6Zr0.4O2 mixed oxides investigated by temperature-programmed reduction and dynamic OSC measurements journal March 2001
Single-atom catalysis of CO oxidation using Pt1/FeOx journal July 2011
The selection of experimental conditions in temperature-programmed reduction experiments
  • Malet, Pilar; Caballero, Alfonso
  • Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases, Vol. 84, Issue 7 https://doi.org/10.1039/f19888402369
journal January 1988
Periodic Operation of Chemical Reactors: a Review journal January 1974
Water Gas Shift Catalysis journal September 2009
Catalytic Properties of Ceria and CeO 2 -Containing Materials journal November 1996
The Water-Gas Shift Reaction journal January 1980
The Scherrer Formula for X-Ray Particle Size Determination journal November 1939
Active Nonmetallic Au and Pt Species on Ceria-Based Water-Gas Shift Catalysts journal August 2003
Dynamic behaviour of automotive catalytic converters subjected to variations in engine exhaust compositions journal December 2005
Structured Perovskite-Based Catalysts and Their Application as Three-Way Catalytic Converters—A Review journal July 2014
Effect of Three Way Conversion Catalyst Operation on the Chemical State of Automotive Sulfur Emissions
  • Cohn, J. G.; Mannion, W. A.; Thompson, C. E.
  • 1975 Automotive Engineering Congress and Exposition, SAE Technical Paper Series https://doi.org/10.4271/750096
conference February 1975