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SCR Deactivation Kinetics for Model-Based Control and Accelerated Aging Applications

Selective Catalytic Reduction (SCR) catalysts are used to reduce NOx emissions from internal combustion engines in a variety of applications [1,2,3,4]. Southwest Research Institute (SwRI) performed an Internal Research & Development project to study SCR catalyst thermal deactivation. The study included a V/W/TiO2 formulation, a Cu-zeolite formulation and a Fe-zeolite formulation. This work describes NH3 storage capacity measurement data as a function of aging time and temperature. Addressing one objective of the work, these data can be used in model-based control algorithms to calculate the current NH3 storage capacity of an SCR catalyst operating in the field, based on time and temperature history. The model-based control then uses the calculated value for effective DEF control and prevention of excessive NH3 slip. Addressing a second objective of the work, accelerated thermal aging of SCR catalysts may be achieved by elevating temperatures above normal operating temperatures.

SCR Deactivation Study for OBD Applications

Selective catalytic reduction (SCR) catalysts will be used to reduce oxides of nitrogen (NOx) emissions from internal combustion engines in a number of applications [1,2,3,4]. Southwest Research Institute® (SwRI)® performed an Internal Research & Development project to study SCR catalyst thermal deactivation. The study included a V/W/TiO2 formulation, a Cu-zeolite formulation and an Fe-zeolite formulation. This work describes NOx timed response to ammonia (NH3) transients as a function of thermal aging time and temperature. It has been proposed that the response time of NOx emissions to NH3 transients, effected by changes in diesel emissions fluid (DEF) injection rate, could be used as an on-board diagnostic (OBD) metric. The objective of this study was to evaluate the feasibility and practicality of this OBD approach.

Evaluation of a NOx Transient Response Method for OBD of SCR Catalysts

OBD requirements for aftertreatment system components require monitoring of the individual system components. One such component can be an NH3-SCR catalyst for NOx reduction. An OBD method that has been suggested is to generate positive or negative spikes in the inlet NH3 concentration, and monitor the outlet NOx transient response. A slow response indicates that the catalyst is maintaining its NH3 storage capacity, and therefore it is probably not degraded. A fast response indicates the catalyst has lost NH3 storage capacity, and may be degraded. The purpose of the work performed at Southwest Research Institute was to assess this approach for feasibility, effectiveness and practicality. The presentation will describe the work performed, results obtained, and implications for applying this method in test laboratory and real-world situations. Presenter Gordon J. Bartley, Southwest Research Institute
Technical Paper

Emissions Reduction Performance of a Bimetallic Platinum/Cerium Fuel Borne Catalyst with Several Diesel Particulate Filters on Different Sulfur Fuels

Results of engine bench tests on a 1998 heavy-duty diesel engine have confirmed the emissions reduction performance of a U.S. Environmental Protection Agency (EPA) registered platinum/cerium bimetallic fuel borne catalyst (FBC) used with several different catalyzed and uncatalyzed diesel particulate filters (DPF's). Performance was evaluated on both a 450ppm sulfur fuel (No.2 D) and a CARB 50ppm low sulfur diesel (LSD) fuel. Particulate emissions of less than 0.02g/bhp-hr were achieved on several combinations of FBC and uncatalyzed filters on 450ppm sulfur fuel while levels of 0.01g/bhp-hr were achieved for both catalyzed and uncatalyzed filters using the FBC with the low sulfur CARB fuel. Eight-mode steady state testing of one filter and FBC combination with engine timing changes produced a 20% nitrogen oxide (NOx) reduction with particulates (PM) maintained at 0.01g/bhp-hr and no increase in measured fuel consumption.
Technical Paper

Performance of Different Cell Structure Converters A Total Systems Perspective

The objective of this effort was to develop an understanding of how different converter substrate cell structures impact tailpipe emissions and pressure drop from a total systems perspective. The cell structures studied were the following: The catalyst technologies utilized were a new technology palladium only catalyst in combination with a palladium/rhodium catalyst. A 4.0-liter, 1997 Jeep Cherokee with a modified calibration was chosen as the test platform for performing the FTP test. The experimental design focused on quantifying emissions performance as a function of converter volume for the different cell structures. The results from this study demonstrate that the 93 square cell/cm2 structure has superior performance versus the 62 square cell/cm2 structure and the 46 triangle cell/cm2 structure when the converter volumes were relatively small. However, as converter volume increases the emissions differences diminish.
Technical Paper

Development of an Ethanol-Fueled Ultra-Low Emissions Vehicle

A 1993 Ford Taurus Flexible Fuel Vehicle (FFV) designed to operate on gasoline or methanol has been modified to run on Ed85 (85 vol.% denatured ethanol, 15 vol.% gasoline) and has demonstrated the ability to meet California's Ultra-Low Emissions Vehicle (ULEV) standards. The vehicle maintains the excellent driveability with potentially increased performance and similar efficiency to the baseline vehicle. Using standard twin OEM catalysts, FTP-75 emissions were 0.085 g/mi NOx, 0.88 g/mi CO, and 0.039 g/mi reactivity-adjusted NMOG. Using close-coupled catalysts upstream of the OEM catalysts, FTP-75 emissions were 0.031 g/mi NOx, 0.297 g/mi CO, and 0.015 g/mi reactivity-adjusted NMOG. The catalysts were aged to about 4,000 miles of equivalent use. These emissions compare with ULEV standards of 0.2 g/mi NOx, 1.7 g/mi CO, and 0.04 g/mi NMOG at 50,000 miles of use.
Technical Paper

Reduced Cold-Start Emissions Using Rapid Exhaust Port Oxidation (REPO) in a Spark-Ignition Engine

An emissions reduction strategy was developed and demonstrated to significantly reduce cold-start hydrocarbon (HC) and CO emissions from a spark ignition (SI), gasoline-fueled engine. This strategy involved cold-starting the engine with an ultra-fuel rich calibration, while metering near-stoichiometric fractions of air directly into the exhaust ports. Using this approach, exhaust constituents spontaneously ignited at the exhaust ports and burned into the exhaust manifold and exhaust pipe leading to the catalytic converter. The resulting exotherm accelerated catalyst heating and significantly decreased light-off time following a cold-start on the FTP-75 with a Ford Escort equipped with a 1.9L engine. Mass emissions measurements acquired during the first 70 seconds of the FTP-75 revealed total-HC and CO reductions of 68 and 50 percent, respectively, when compared to baseline measurements.
Technical Paper

An Integrated Engine Cycle Simulation Model with Species Tracking in Piping System

Due to compressibility, reactivity, evaporation and mixing, the gas species concentration varies significantly along the intake and exhaust pipes of an engine. An understanding of this behavior is vital to correctly predict catalyst performance because the behavior of a catalyst very much depends on the instantaneous local species concentrations, rather than those in the cylinder. Also, knowing this behavior is more important to assess the effects of exhaust gas recirculation (EGR). The objective of this research is to develop a tool that is capable of predicting the instantaneous species concentration throughout the entire intake and exhaust system, and to lay out a foundation to model catalysts in the near future. This is done by first developing a complete engine cycle simulation model that is able to accurately predict wave dynamics in the piping system. Then, species tracking is accomplished by solving the species conservation equations.
Technical Paper

EGR System Integration on a Pump Line-Nozzle Engine

The minimum oxides of nitrogen (NOx) emissions over the U.S. Federal Test Procedure (FTP) using exhaust gas recirculation (EGR) were investigated on a heavy-duty diesel engine featuring a pump-line-nozzle fuel injection system. Due to the technical merits of electronic fuel injection systems, most accounts of EGR system development for heavy-duty diesel engines have focused on these types of engines and not engines with mechanical fuel systems. This work details use of a high-pressure-loop EGR configuration and a novel, computer-controlled, EGR valve that allowed for optimizing the EGR rate as a function of speed and load on a 6L, turbo-charged/intercooled engine. Cycle NOx levels were reduced nearly 50 percent to 2.3 g/hp-hr using conventional diesel fuel and application of only EGR, but particulates increased nearly three-fold even with the standard oxidation catalyst employed.
Technical Paper

Development of a Lean-NOx Catalyst Containing Metal-Ligand Complex Impregnated Molecular Sieves

This paper describes the development and evaluation of an operative catalyst for the reduction of NOx in lean exhaust. A catalyst that incorporates iron (II)-complex impregnated modified mesoporous molecular sieves (MCM-41) has been synthesized and further treated with [pd(NH3)4]Cl2 [1]. Experimental results suggest a hydrocarbon-independent reduction of NOx takes place on the iron center, and oxidation of CO is assisted by the palladium ion. The catalytic activity toward HC CO, and NOx removal was studied with simulated and real engine exhaust in the laboratory and on an engine, respectively. Engine test results demonstrate a reduction of NOx of up to 10 percent at catalyst inlet temperatures in the range of 260°C to 280°C. In this paper, possible NOx reduction pathways are also discussed.
Technical Paper

An Intake Charge Cooling System for Application to Diesel, Gasoline and Natural Gas Engines

Low intake manifold temperature, well below ambient, has many applications in internal combustion engines. In diesel engines, it can reduce NOx to a level of 2.0 g/hp-hr or below, going beyond the 1994 heavy duty diesel engine emissions standards. In gasoline engines, it can allow high compression ratio, turbocharged operation without end gas knock. This will permit ready conversion of some heavy duty diesel engines to gasoline operation at increased power density and lower emissions. In natural gas engines, it will allow base diesel engine to be converted to stoichiometric natural gas operation without increasing thermal loads. A three way catalyst can then be used to reduce emissions.
Technical Paper

Formaldehyde Emission Control Technology for Methanol-Fueled Vehicles: Catalyst Selection

The use of methanol as a “clean fuel” appears to be a viable approach to reduce air pollution. However, concern has been expressed about potentially high formaldehyde emissions from stoichiometrically operated light-duty vehicles. This paper presents results from an emission test program conducted for the California Air Resources Board (CARB) and the South Coast Air Quality Management District (SCAQMD) to identify and evaluate advanced catalyst technology to reduce formaldehyde emissions without compromising regulated emission control. An earlier paper presented the results of evaluating eighteen different catalyst systems on a hybrid methanol-fueled test vehicle. (1)* This paper discusses the optimization of three of these catalyst systems on four current technology methanol-fueled vehicles. Emission measurements were conducted for formaldehyde, nonmethane organic gases (NMOG), methanol, carbon monoxide, and oxides of nitrogen emissions.
Technical Paper

Emission Control Strategies for Small Utility Engines

Recent approval of emission standards for small utility engines by the California Air Resources Board(1)* suggests that substantial reductions in emissions from small utility engines will soon be required. While 1994 standards may be met with simple engine adjustments or modifications, 1999 standards are much more stringent and may require the use of catalysts in conjunction with other emission reduction technologies. Assessing the feasibility of candidate emission control strategies is an important first step. Various emission reduction technologies were applied to three different 4-stroke engines. Emission tests were conducted to determine the effectiveness of air/fuel ratio changes, thermal oxidation, exhaust gas recirculation, and catalytic oxidation with and without supplemental air. Results of these evaluations, along with implications for further work, are presented. One engine's emissions were reduced below the levels of 1999 ARB standards.
Technical Paper

Lean NOx Catalyst Evaluation and Characterization

Copper ion exchange procedures were used to prepare zeolite-based catalysts for NOx reduction in lean (oxygen-rich) exhaust. Energy dispersive x-ray fluorescence and scanning electron microscopy analyses confirmed the presence of copper in the zeolite matrix. Zeolites were applied onto honeycomb and foam substrates, and evaluated for catalytic NOx reduction efficiency using engine exhaust. Copper-exchanged zeolite catalysts prepared for this study revealed NOx reduction of 95 percent for a period of seven minutes using previously adsorbed exhaust hydrocarbons as the reducing agent. Experiments using ethylene injection to supplement the exhaust suggest long-term and sustained NOx reduction, initially observed at 52 percent. Experimental results and performance comparisons of ZSM-5, mordenite, and Y-type zeolites are discussed. Zeolite catalysts based on Cu-mordenite showed high levels of initial NOx reduction, while results using Cu-ZSM-5 suggested better long-term activity.
Technical Paper

Fuel Effects on Emissions from an Advanced Technology Vehicle

A 1991 Toyota Camry equipped with an electrically-heated catalyst (EHC) system was evaluated in duplicate over the Federal Test Procedure (FTP) with three different fuels. Evaluations were conducted with the EHC in place but without any external heating, and with the EHC operated with a post-crank heating strategy. The EHC system was placed immediately upstream of an original production catalyst, which was then moved to a location 40.6 cm from the exhaust manifold. The three test fuels were: 1) the Auto/Oil industry average gasoline, RF-A; 2) a fuel meeting California's Phase II gasoline specifications; and 3) a paraffinic test fuel. Non-methane organic gas (NMOG) emission rates with the EHC active were similiar with all three fuels, with absolute levels less than or equal to California's 50,000 mile Ultra-Low Emission Vehicle (ULEV) standard. Substantial differences, however were observed in the ozone forming potential of these fuels with the EHC active.
Technical Paper

Natural Gas Converter Performance and Durability

Natural gas-fueled vehicles impose unique requirements on exhaust aftertreatment systems. Methane conversion, which is very difficult for conventional automotive catalysts, may be required, depending on future regulatory directions. Three-way converter operating windows for simultaneous conversion of HC, CO, and NOx are considerably more narrow with gas engine exhaust. While several studies have demonstrated acceptable fresh converter performance, aged performance remains a concern. This paper presents the results of a durability study of eight catalytic converters specifically developed for natural gas engines. The converters were aged for 300 hours on a natural gas-fueled 7.0L Chevrolet engine operated at net stoichiometry. Catalyst performance was evaluated using both air/fuel traverse engine tests and FTP vehicle tests. Durability cycle severity and a comparison of results for engine and vehicle tests are discussed.
Technical Paper

Achieving Fast Catalyst Light-Off from a Heavy-Duty Stoichiometric Natural Gas Engine Capable of 0.02 g/bhp-hr NOX Emissions

Recently conducted work has been funded by the California Air Resources Board (CARB) to explore the feasibility of achieving 0.02 g/bhp-hr NOX emissions for heavy-duty on-road engines. In addition to NOX emissions, greenhouse gas (GHG), CO2 and methane emissions regulations from heavy-duty engines are also becoming more stringent. To achieve low cold-start NOX and methane emissions, the exhaust aftertreatment must be brought up to temperature quickly while keeping proper air-fuel ratio control; however, a balance between catalyst light-off and fuel penalty must be addressed to meet future CO2 emissions regulations. This paper details the work executed to improve catalyst light-off for a natural gas engine with a close-coupled and an underfloor three-way-catalyst while meeting an FTP NOX emission target of 0.02 g/bhp-hr and minimizing any fuel penalty.
Technical Paper

Solid Particle Number and Ash Emissions from Heavy-Duty Natural Gas and Diesel w/SCRF Engines

Solid and metallic ash particle number (PN) and particulate matter (PM) mass emission measurements were performed on a heavy-duty (HD) on-highway diesel engine and a compressed natural gas (CNG) engine. Measurements were conducted under transient engine operation that included the FTP, WHTC and RMC. Both engines were calibrated to meet CARB ultra low NOX emission target of 0.02 g/hp-hr, a 90% reduction from current emissions limit. The HD diesel engine final exhaust configuration included a number of aftertreatement sub-systems in addition to a selective catalytic reduction filter (SCRF). The stoichiometric CNG engine final configuration included a closed coupled Three Way Catalyst (ccTWC) and an under floor TWC (ufTWC). The aftertreatment systems for both engines were aged for a full useful life (FUL) of 435,000 miles, prior to emissions testing. PM mass emissions from both engines were comparable and well below the US EPA emissions standard.
Technical Paper

Identifying Limiters to Low Temperature Catalyst Activity

The drive to more fuel efficient vehicles is underway, with passenger car targets of 54.5 mpg fleet average by 2025. Improving engine efficiency means reducing losses such as the heat lost in the exhaust gases. However, reducing exhaust temperature makes it harder for emissions control catalysts to function because they require elevated temperatures to be active. Addressing this conundrum was the focus of the work performed. The primary objective of this work was to identify low temperature limiters for a variety of catalyst aftertreatment types. The ultimate goal is to reduce catalyst light-off temperatures, and the knowledge needed is an understanding of what prevents a catalyst from lighting off, why, and how it may be mitigated. Collectively these are referred to here as low temperature limiters to catalyst activity.
Technical Paper

Emissions Control of Gasoline Engines for Heavy-Duty Vehicles

This paper summarizes an investigation of reductions in exhaust emission levels attainable using various techniques appropriate to gasoline engines used in vehicles over 14,000 lbs GVW. Of the eight gasoline engines investigated, two were evaluated parametrically resulting in an oxidation and reduction catalyst “best combination” configuration. Four of the engines were evaluated in an EGR plus oxidation catalyst configuration, and two involved only baseline tests. Test procedures used in evaluating the six “best combination” configurations include: three engine emission test procedures using an engine dynamometer, a determination of vehicle driveability, and two vehicle emission test procedures using a chassis dynamometer. Dramatic reductions in emissions were attained with the catalyst “best combination” configurations. Engine durability, however, was not investigated.