Winthrop F. Watts

Diesel Aerosol Sampling in the Atmosphere

The University of Minnesota Center for Diesel Research along with a research team including Caterpillar, Cummins, Carnegie Mellon University, West Virginia University (WVU), Paul Scherrer Institute in Switzerland, and Tampere University in Finland have performed measurements of Diesel exhaust particle size distributions under real-world dilution conditions. A mobile aerosol emission laboratory (MEL) equipped to measure particle size distributions, number concentrations, surface area concentrations, particle bound PAHs, as well as CO 2 and NO x concentrations in real time was built and will be described. The MEL was used to follow two different Cummins powered tractors, one with an older engine (L10) and one with a state-of-the-art engine (ISM), on rural highways and measure particles in their exhaust plumes. This paper will describe the goals and objectives of the study and will describe representative particle size distributions observed in roadway experiments with the truck powered by the ISM engine.

Real-time characterization of ultrafine and accumulation mode particles in ambient combustion aerosols

Abstract The diffusion charging sensor (DC), photoelectric aerosol sensor (PAS) and condensation particle counter (CPC) are real-time particle instruments that have time resolutions s and are suitable for field use. This paper shows how the relative fraction of nuclei mode particles (D⩽50 nm ) in ambient combustion aerosols can be determined, along with the coverage degree of the respective accumulation mode particles with a modal diameter of ∼100 nm . Main tools for interpretation are the diameter of average surface D Ave, S (obtained from CPC and DC measurements) and PAS/DC versus D Ave, S scatter plots. Compared to the scanning mobility particle sizer (SMPS), which is a standard instrument for aerosol particle size distribution measurements, the presented method has a limited accuracy, but is substantially faster. Additionally, it is experimentally less demanding than SMPS measurements, especially for field applications.

On-Road Exposure to Highway Aerosols. 1. Aerosol and Gas Measurements

On-road experiments were conducted to determine the sensitivities of rats to real-world aerosol. This article summarizes the on-road aerosol and gas measurements and provides background information for the companion paper on the rat exposures. Measurements were carried out over 10 days, 6 h/day, driving a route from Rochester to Buffalo. Aerosol instrumentation used in this study included two scanning mobility particle sizers (SMPS) to determine the aerosol size distribution from 10 to 300 nm, 2 stand-alone condensation particle counters to determine the total aerosol number concentration, and an electrical aerosol detector to determine the aerosol length concentration. A thermal denuder (TD) was used with one of the SMPS instruments to determine the size distribution of the non-volatile fraction. Filter samples were collected and analyzed for elemental carbon, and gas analyzers measured ambient levels of CO, CO2, and NO. Average daily total aerosol number concentration ranged from 200,000 to 560,000 particles/cm3. Past studies on urban highways have measured total number concentrations ranging between 104 and 106 particles/cm3. The average daily NO concentration ranged from 0.10 to 0.24 ppm and the corresponding CO2 concentration ranged from 400 to 420 ppm. The average daily geometric number mean particle size determined by the SMPS ranged from 15 to 20 nm. The TD reduced the average SMPS number concentration between 87 and 95% and the SMPS volume between 54 and 83%, suggesting that most of the particles consisted of volatile material. The TD also increased the geometric number mean diameter from 15 to 20 nm to 30 to 40 nm.

Effects of on-road highway aerosol exposures on autonomic responses in aged, spontaneously hypertensive rats.

Epidemiological studies associate ambient particulate pollution with adverse health outcomes in elderly individuals with cardiopulmonary diseases. We hypothesized that freshly generated ultrafine particles (UFP) contribute to these effects, as they are present in high number concentrations on highways and vehicle passengers are exposed directly to them. Aged spontaneously hypertensive rats (9–12 mo) with implanted radiotelemetry devices were exposed to highway aerosol or filtered, gas-denuded (clean) air using an on-road exposure system to examine effects on heart rate (HR) and heart-rate variability (HRV). On the day of exposure, rats were pretreated with low-dose inhaled or injected lipopolysaccharide (LPS) to simulate respiratory tract or systemic inflammation, respectively. Exposures (6 h) in compartmentalized whole-body chambers were performed in an air conditioned compartment of a mobile laboratory on I-90 between Rochester and Buffalo, NY. HRV parameters were calculated from telemetric blood pressure signals and analyzed for the baseline period and for the first 32 h postexposure. The aerosol size (count median diameter = 15–20 nm; geometric standard deviation = 1.4–4.3) and number concentration (1.95–5.62 × 105/cm3) indicated the predominance of UFP. Intraperitoneal LPS significantly affected all of the parameters in a time-dependent manner; response patterns after inhaled or injected LPS pretreatment were similar, but more prolonged and greater in LPS-injected rats. A significant effect of highway aerosol was found, irrespective of pretreatment, which resulted in decreased HR in comparison to clean air-exposed rats. This effect was more persistent (∼ 14 h) in those rats that received ip LPS as compared to saline. The highway aerosol also significantly affected short-term alterations in autonomic control of HR, as evidenced by elevations in normalized high frequency power and decreased vagosympathetic balance. These findings show that environmental exposure concentrations of mixed traffic-related UFP/gas-phase emissions can affect the autonomic nervous system.

On-Road Exposure to Highway Aerosols. 2. Exposures of Aged, Compromised Rats

Ambient particulate pollution is associated with adverse health effects in epidemiological studies of the elderly with cardiopulmonary diseases. We hypothesize that ultrafine particles (UFP) contribute to these effects, especially when they are freshly generated and occur at high number concentrations. Studies to determine adverse effects have been performed using laboratory-generated surrogates, diluted exhaust from stationary engines, or concentrated ambient UFPs. Methodological difficulties exist with such experiments, and questions remain about how well these particles model those found in ambient air. Freshly generated UFPs are present at high concentrations on highways and vehicle passengers are directly exposed to them. We wished to expose rats to these UFPs to test their potential to cause effects. Since such exposures have not been done before, one objective of our study was to demonstrate the feasibility of an on-road exposure study. Secondly, we wished to determine if there are significant exposure-related effects in aged, compromised rats. Old rats (21-mo F-344) were exposed directly on highways to either the aerosol (< 1 μm)/gas phase, gas phase only, or filtered air using an on-road exposure system. Some rats were pretreated with a low dose of inhaled endotoxin or with instilled influenza virus to induce lung inflammation. The exposures in compartmentalized whole-body chambers consisted of 6-h driving periods on I-90 between Rochester and Buffalo once or 3 days in a row. Endpoints related to lung inflammation, inflammatory cell activation, and acute-phase responses were measured after exposure. The on-road exposure system did not affect measured endpoints in filtered air-exposed rats, indicating that it was well tolerated by them. We observed the expected increases in response (inflammation, inflammatory cell activation) to the priming agents. We also found a significant particle-associated increase in plasma endothelin-2, suggesting alterations in vascular endothelial cell activation. In addition, we observed main effects of particles related to the acute-phase response and inflammatory-cell activation. Interactions between on-road particles and the priming agents were also found. These results suggest that exposures to on-road particle mixtures have effects on the pulmonary and cardiovascular system in compromised, old rats. Furthermore, they demonstrate that on-road exposures are feasible and could be performed in future studies with more continuous particle exposures.

Impact of Ambient Temperatures and Driving Conditions on the Chemical Composition of Particulate Matter Emissions from Non-Smoking Gasoline-Powered Motor Vehicles

The detailed chemical composition of particulate matter emissions from four non-smoking gasoline powered motor vehicles were measured using three different driving conditions: a cold-cold start Unified Driving Cycle (UDC), a hot UDC, and a steady state cruise driving cycle. The cold-cold start UDC tests were performed with a cold-cold start temperature of 0°C, which is significantly lower than the 24°C cold start temperature widely used for motor vehicle testing. Each vehicle was operated over three cold-cold UDC cycles, three hot UDC cycles, and a steady state driving cycle comprised of 2 hours at 100 kilometers per hour (kph) plus 1 hour at 50 kph. Particulate matter emissions were characterized for elemental carbon (EC), organic carbon (OC), sulfate ions, nitrate ions, ammonium ions, and organic compounds using gas chromatography mass spectrometry (GCMS). Mass emissions rates for the test vehicles using both the hot UDC and steady state driving cycles ranged from < 0.1 to 1.3 mg km −1 , while the average cold-cold UDC cycle emissions ranged from 1.0 to 7.1 mg km −1 for the four vehicles. The cold-cold start UDC emissions averaged 5–30 times higher than the hot start UDC emissions. EC was an important contributor to the particulate matter emissions for the cold-cold start UDC emissions. Speciation of the organic compounds in the particulate matter emissions demonstrates differences in the composition of the organic aerosol emissions for the different driving cycles. The results of the present study demonstrate the important impact of cold-cold start temperature and driving conditions.

Driving down on-highway particulate emissions

It has been reported that particulate emissions from diesel vehicles could be associated with damaging human health, global warming and a reduction in air quality. These particles cover a very large size range, typically 3 to 10 000 nm. Filters in the vehicle exhaust systems can substantially reduce particulate emissions but until very recently it was not possible to directly characterise actual on-road emissions from a vehicle. This paper presents the first study of the effect of filter systems on the particulate emissions of a heavy-duty diesel vehicle during real-world driving. The presence of sulfur in the fuel and in the engine lubricant can lead to significant emissions of sulfate particles < 30 nm in size (nanoparticles). We have demonstrated that when using low sulfur fuel in combination with a uniquely formulated low sulfur lubricant and a suitable filter system that the particulate emissions of a heavy-duty vehicle were reduced to the levels already present in the ambient environment. PM EMISSIONS AND DIESEL PARTICULATE FILTER (DPF) TECHNOLOGY Diesel Particulate Matter (PM) consists primarily of carbonaceous soot and a Volatile Organic Fraction (VOF) composed mainly of hydrocarbons with lesser amounts of nitrate and sulfate species. It is becoming increasingly recognised that PM emissions from dieselpowered vehicles may have adverse environmental effects. For example, it was proposed that the elemental carbon fraction can increase global warming effects. In addition, the medical community is closely examining the effects of PM on human health as a function of particle size. Reports in scientific literature suggest that there is a link between environmental exposure to fine particles less than 2.5 m in size to adverse health effects. These studies elucidated a range of causal mechanisms but have not developed a quantitative understanding of their relative importance. Studies that are more recent investigated the hypothesis that ultrafine particles <100 nm in size are detrimental to human health. It has also been reported that the relationship between ultrafine particles and health may be at least partially due to the high efficiency of particle deposition in the respiratory tract for the very small particles (Alveolar deposition is highest for particles approximately 20 nm in size). Regulatory agencies such as the U.S. Environmental Protection Agency (EPA) have adopted mass-based air pollution regulations for particulate matter. Other metrics, such as particle number or surface area, may be more important in characterising the physical properties of aerosol related to health effects. Figure 1 illustrates relationships between combustion aerosol number, surface area and mass weighted size distributions. In this case the distribution typifies a diesel aerosol distribution. The shape of the aerosol size distribution from a spark ignition engine would be similar but with relatively less material in the accumulation mode region. 2006-01-0916 Driving Down On-Highway Particulate Emissions D. B. Kittelson, W. F. Watts and J. P. Johnson University of Minnesota, Department of Mechanical Engineering

Reducing motor vehicle greenhouse gas emissions in a non-California state: a case study of Minnesota.

Approaches for reducing greenhouse gas (GHG) emissions from motor vehicles include more-efficient vehicles, lower-carbon fuels, and reducing vehicle-kilometers traveled (VKT). Many U.S. states are considering steps to reduce emissions through actions in one or more of these areas. We model several technology and policy options for reducing GHGs from motor vehicles in Minnesota. Considerable analysis of transportation GHGs has been done for California, which has a large population and vehicle fleet and can enact unique emissions regulations; Minnesota represents a more typical state with respect to many demographic and transportation parameters. We conclude that Minnesota has a viable approach to meeting its stated GHG reduction targets (15% by 2015 and 30% by 2025, relative to year 2005) only if advancements are made in all three areas-vehicle efficiency, carbon content of fuels, and VKT. If policies focus on only one or two areas, potential improvements may be negated by backsliding in another area (e.g., increasing VKT offsetting improvements in vehicle efficiency).

Filtration Efficiency and Pressure Drop of Miniature Diesel Particulate Filters

A method was developed to evaluate miniature diesel particulate filters (DPFs). To validate the performance of the instrumentation and test apparatus, measurements were made using silicon carbide (SiC) and cordierite miniature filters with representative microstructures. Filtration efficiency (FE), the most penetrating particle size (MPPS), and pressure drop were measured for catalyzed and uncatalyzed advanced ceramic material (ACM) acicular mullite and representative commercial filters to determine the impact of substrate morphology, the formation of a soot cake, and the presence of a catalyst coating on filtration properties. FE measurements demonstrated that filter geometry and microstructure significantly influence initial filtration performance. ACM filters had high initial FE and the MPPS near ∼200 nm. Reduction of the ACM pore size in the absence of a reduction in porosity increased initial FE even more, but its influence on MPPS was not resolvable. The presence of a catalyst and washcoat on the ACM increased the pressure drop but increased initial FE and reduced MPPS to <100 nm. The addition of a washcoat allowed the rapid buildup of a soot cake, which resulted in a more rapid rate of increase in FE compared to uncatalyzed ACM. The similarity in the ACM and cordierite soot cakes after a long loading time is consistent with theory that suggests the formation of the soot cake depends primarily on the Péclet (Pe) number, which is influenced only by macroscopic filter geometry and prevailing test conditions. Copyright 2013 American Association for Aerosol Research

Alternatives to the Gravimetric Method for Quantification of Diesel Particulate Matter near the Lower Level of Detection

Abstract This paper is part of the Journal of the Air & Waste Management Association’s 2010 special issue on combustion aerosol measurements. The issue is a combination of papers that synthesize and evaluate ideas and perspectives that were presented by experts at a series of workshops sponsored by the Coordinating Research Council that aimed to evaluate the current and future status of diesel particulate matter (DPM) measurement. Measurement of DPM is a complex issue with many stakeholders, including air quality management and enforcement agencies, engine manufacturers, health experts, and climatologists. Adoption of the U.S. Environmental Protection Agency 2007 heavy-duty engine DPM standards posed a unique challenge to engine manufacturers. The new standards reduced DPM emissions to the point that improvements to the gravimetric method were required to increase the accuracy and the sensitivity of the measurement. Despite these improvements, the method still has shortcomings. The objectives of this paper are to review the physical and chemical properties of DPM that make gravimetric measurement difficult at very low concentrations and to review alternative metrics and methods that are potentially more accurate, sensitive, and specific. Particle volatility, size, surface area, and number metrics are considered, as well as methods to quantify them. Although the authors believe that an alternative method is required to meet the needs of engine manufacturers, the methods reviewed in the paper are applicable to other areas where the gravi-metric method detection limit is approached and greater accuracy and sensitivity are required. The paper concludes by suggesting a method to measure active surface area, combined with a method to separate semi-volatile and solid fractions to further increase the specificity of the measurement, has potential for reducing the lower detection limit of DPM and enabling engine manufacturers to reduce DPM emissions in the future.