Biomedical subjects

Philip K Hopke

Publications and source records attributed to Philip K Hopke.

32 records · Page 2Linked to original sources

PubMed2005

Estimation of organic carbon blank values and error structures of the speciation trends network data for source apportionment.

Because the particulate organic carbon (OC) concentrations reported in U.S. Environment Protection Agency Speciation Trends Network (STN) data were not blank corrected, the OC blank concentrations were estimated using the intercept in particulate matter < or = 2.5 microm in aerodynamic diameter (PM2.5) regression against OC concentrations. The estimated OC blank concentrations ranged from 1 to 2.4 microg/m3 showing higher values in urban areas for the 13 monitoring sites in the northeastern United States. In the STN data, several different samplers and analyzers are used, and various instruments show different method detection limit (MDL) values, as well as errors. A comprehensive set of error structures that would be used for numerous source apportionment studies of STN data was estimated by comparing a limited set of measured concentrations and their associated uncertainties. To examine the estimated error structures and investigate the appropriate MDL values, PM2.5 samples collected at a STN site in Burlington, VT, were analyzed through the application of the positive matrix factorization. A total of 323 samples that were collected between December 2000 and December 2003 and 49 species based on several variable selection criteria were used, and eight sources were successfully identified in this study with the estimated error structures and min values among different MDL values from the five instruments: secondary sulfate aerosol (41%), secondary nitrate aerosol (20%), airborne soil (15%), gasoline vehicle emissions (7%), diesel emissions (7%), aged sea salt (4%), copper smelting (3%), and ferrous smelting (2%). Time series plots of contributions from airborne soil indicate that the highly elevated impacts from this source were likely caused primarily by dust storms.

Air Pollutants↗

PubMed2005

Improving source apportionment of fine particles in the eastern United States utilizing temperature-resolved carbon fractions.

The objectives of this study were to examine the use of carbon fractions to identify particulate matter (PM) sources, especially traffic-related carbonaceous particle sources, and to estimate their contributions to the particle mass concentrations. In recent studies, positive matrix factorization (PMF) was applied to ambient fine PM (PM2.5) compositional data sets of 24-hr integrated samples including eight individual carbon fractions collected at three monitoring sites in the eastern United States: Atlanta, GA, Washington, DC, and Brigantine, NJ. Particulate carbon was analyzed using the Interagency Monitoring of Protected Visual Environments/Thermal Optical Reflectance method that divides carbon into four organic carbons (OC): pyrolized OC and three elemental carbon (EC) fractions. In contrast to earlier PMF studies that included only the total OC and EC concentrations, gasoline emissions could be distinguished from diesel emissions based on the differences in the abundances of the carbon fractions between the two sources. The compositional profiles for these two major source types show similarities among the three sites. Temperature-resolved carbon fractions also enhanced separations of carbon-rich secondary sulfate aerosols. Potential source contribution function analyses show the potential source areas and pathways of sulfate-rich secondary aerosols, especially the regional influences of the biogenic, as well as anthropogenic secondary aerosol. This study indicates that temperature-resolved carbon fractions can be used to enhance the source apportionment of ambient PM2.5.

Air Pollutants, Occupational↗

PubMed2005

Workgroup report: workshop on source apportionment of particulate matter health effects--intercomparison of results and implications.

Although the association between exposure to ambient fine particulate matter with aerodynamic diameter < 2.5 microm (PM2.5) and human mortality is well established, the most responsible particle types/sources are not yet certain. In May 2003, the U.S. Environmental Protection Agency's Particulate Matter Centers Program sponsored the Workshop on the Source Apportionment of PM Health Effects. The goal was to evaluate the consistency of the various source apportionment methods in assessing source contributions to daily PM2.5 mass-mortality associations. Seven research institutions, using varying methods, participated in the estimation of source apportionments of PM2.5 mass samples collected in Washington, DC, and Phoenix, Arizona, USA. Apportionments were evaluated for their respective associations with mortality using Poisson regressions, allowing a comparative assessment of the extent to which variations in the apportionments contributed to variability in the source-specific mortality results. The various research groups generally identified the same major source types, each with similar elemental makeups. Intergroup correlation analyses indicated that soil-, sulfate-, residual oil-, and salt-associated mass were most unambiguously identified by various methods, whereas vegetative burning and traffic were less consistent. Aggregate source-specific mortality relative risk (RR) estimate confidence intervals overlapped each other, but the sulfate-related PM2.5 component was most consistently significant across analyses in these cities. Analyses indicated that source types were a significant predictor of RR, whereas apportionment group differences were not. Variations in the source apportionments added only some 15% to the mortality regression uncertainties. These results provide supportive evidence that existing PM2.5 source apportionment methods can be used to derive reliable insights into the source components that contribute to PM2.5 health effects.

Air Pollutants↗

PubMed2004

Characteristics of nucleation and growth events of ultrafine particles measured in Rochester, NY.

Number concentrations and size distributions of particles in the size range of 0.010-0.500 microm were measured in Rochester, NY, from December 2001 to December 2002. The relationships between the number concentrations, gaseous pollutants, and meteorological parameters were examined during particle nucleation events. More than 70% of measured total number concentration was associated with ultrafine particles (UFP, 0.011-0.050 microm). Morning nucleation events typically peaking UFP number concentrations at around 08:00 were apparent in winter months with CO increases. These particles appear to be formed following direct emissions from motorvehicles during morning rush hour. There were also often observed increases in this smaller-sized range particles in the late afternoon during the afternoon rush hour, particularly in winter when the mixing heights remain lowerthan in summer. Strong afternoon nucleation events (> 30,000 cm(-3)) peaking at around 13: 00 were more likely to occur in spiring and summer months. During the prominent nucleation events, peaks of SO2 were strongly associated with the number concentrations of UFP, whereas there were no significant correlations between these events and PM2.5 and CO. Increased SO2 concentrations were observed when the wind direction was northwesterly where three SO2 sources were located. It is hypothesized that UFP formed during the events are sulfuric acid and water from the oxidation of SO2. There were also a more limited number of nucleation events followed by particle growth up to approximately 0.1 microm over periods of up to 18 h. The nucleation and growth events tended to be common in spring months especially in April.

Air Pollutants↗

PubMed2004

Source identification of volatile organic compounds in Houston, Texas.

The complexity of the volatile organic compound (VOC) mixture in the Houston area makes studies of the air quality in that area very challenging. In this paper, a novel factor analysis model, where the normal chemical mass balance model was augmented by a parallel equation that accounted for wind speed and direction, temperature, and weekend/weekday effects, was fitted with a multilinear engine (ME) to provide identification and apportionment of the VOC sources at the La Porte Municipal Airport site in Houston during the Texas Air Quality Study (TexAQS) 2000. The analysis determined the profiles and contributions of nine sources and the corresponding wind speed, wind direction, temperature, and weekend factors. The reasonableness of these results not only suggests the high resolving power of the expanded factor analysis model for source apportionment but also provides the novel and effective auxiliary information for more specific source identification. In addition, a new approach to estimate the measurement uncertainty and the details of determining the source number and dealing with missing values are also presented as important parts of the data analysis process. This study demonstrates the feasibility of the expanded model to identify sources in complex VOC systems and extract useful information for locating VOC emitters and controlling their emissions in the Houston area.

Air Pollutants↗

PubMed2004

Multilinear model for spatial pattern analysis of the Measurement of Haze and Visual Effects project.

A multilinear model was developed for the analysis of the spatial patterns and possible sources affecting haze and its visual effects in the southwestern United States. The data from the project Measurement of Haze and Visual Effects (MOHAVE) collected during the late winter and mid-summer of 1992 at the monitoring sites in four states (i.e., California, Arizona, Nevada and Utah) were used in the study. The three-way data array was analyzed by a four-product-term model. This study makes a direct effort to include wind patterns as a component in the model in order to obtain the information of the spatial patterns of source contributions. The solution is computed using the conjugate gradient algorithm with applied non-negativity constraints. For the winter data set, reasonable solutions contained six sources and six wind patterns. The analysis of summer data required seven sources and seven wind patterns. The ME results are compared to the prior single-species empirical orthogonal function analysis results--and prior work describing the transport pathways.

Air Pollutants↗

PubMed2004

Analysis of ambient particle size distributions using Unmix and positive matrix factorization.

Hourly averaged particle size distributions measured at a centrally located urban site in Seattle were analyzed through the application of bilinear positive matrix factorization (PMF) and Unmix to study underlying size distributions and their daily patterns. A total of 1051 samples each with 16 size intervals from 20 to 400 nm were obtained from a differential mobility particle sizer operating between December 2000 and February 2001. Both PMF and Unmix identify four similar underlying factors in the size distributions. Factor 1 is an accumulation mode particle size spectrum that shows a regular nocturnal pattern, and factor 2 is a larger particle distribution. Factor 3 is assigned as a traffic-related particle distribution, based on its correlations with accompanying gas-phase measurements, and has a regular weekday-high rush-hour pattern. Factor 4 is a traffic-related particle size distribution that has a regular rush-hour pattern on weekdays as well as weekends. Conditional probability functions (CPF) were computed using wind profiles and factor contributions. The results of CPF analysis suggest that these factors are correlated with surrounding particle sources of wood burning, secondary aerosol, diesel emissions, and motor vehicle emissions.

Aerosols↗

PubMed2004

Source apportionment of fine particles in Washington, DC, utilizing temperature-resolved carbon fractions.

Integrated ambient particulate matter < or =2.5 microm in aerodynamic diameter (PM2.5) samples were collected at a centrally located urban monitoring site in Washington, DC, on Wednesdays and Saturdays using Interagency Monitoring of Protected Visual Environments samplers. Particulate carbon was analyzed using the thermal optical reflectance method that divides carbon into four organic carbon fractions, pyrolyzed organic carbon, and three elemental carbon fractions. A total of 35 variables measured in 718 samples collected between August 1988 and December 1997 were analyzed. The data were analyzed using Positive Matrix Factorization and 10 sources were identified: sulfate (SO4(2-))-rich secondary aerosol I (43%), gasoline vehicle (21%), SO4(2-)-rich secondary aerosol II (11%), nitrate-rich secondary aerosol (9%), SO4(2-)-rich secondary aerosol III (6%), incinerator (4%), aged sea salt (2%), airborne soil (2%), diesel emissions (2%), and oil combustion (2%). In contrast to a previous study that included only total organic carbon and elemental carbon fractions, motor vehicles were separated into fractions identified as gasoline vehicle and diesel emissions containing carbon fractions whose abundances were different between the two sources. This study indicates that the temperature-resolved carbon fraction data can be utilized to enhance source apportionment, especially with respect to the separation of diesel emissions from gasoline vehicle sources. Conditional probability functions using surface wind data and deduced source contributions aid in the identifications of local sources.

Air Pollutants↗

PubMed2004

Measurement of ultrafine particle size distributions from coal-, oil-, and gas-fired stationary combustion sources.

Currently, we have limited knowledge of the physical and chemical properties of emitted primary combustion aerosols and the changes in those properties caused by nucleation, condensation growth of volatile species, and particle coagulations under dilution and cooling in the ambient air. A dilution chamber was deployed to sample exhaust from a pilot-scale furnace burning various fuels at a nominal heat input rate of 160 kW/h(-1) and 3% excess oxygen. The formation mechanisms of particles smaller than 420 nm in electrical mobility diameter were experimentally investigated by measurement with a Scanning Mobility Particle Sizer (SMPS) as a function of aging times, dilution air ratios, combustion exhaust temperatures, and fuel types. Particle formation in the dilution process is a complex mixture of nucleation, coagulation, and condensational growth, depending on the concentrations of available condensable species and solid or liquid particles (such as soot, ash) in combustion exhausts. The measured particle size distributions in number concentrations measured show peaks of particle number concentrations for medium sulfur bituminous coal, No. 6 fuel oil, and natural gas at 40-50 nm, 70-100 nm, and 15-25 nm, respectively. For No. 6 fuel oil and coal, the particle number concentration is constant in the range of a dilution air ratio of 50, but the number decreases as the dilution air ratio decreases to 10. However, for natural gas, the particle number concentration is higher at a dilution air ratio of 10 and decreases at dilution air ratios of 20-50. At a dilution air ratio of 10, severe particle coagulation occurs in a relatively short time. Samples taken at different combustion exhaust temperatures for these fuel types show higher particle number concentrations at 645 K than at 450 K. As the aging time of particles increases, the particles increase in size and the number concentrations decrease. The largest gradient of particle number distribution occurs within the first 10 sec after dilution but shows only minor differences between 10 and 80 sec. The lifetimes of the ultrafine particles are relatively short, with a scale on the order of a few seconds. Results from this study suggest that an aging time of 10 sec and a dilution air ratio of 20 are sufficient to obtain representative primary particle emission samples from stationary combustion sources.

Aerosols↗

PubMed2003

Advanced factor analysis of spatial distributions of PM2.5 in the eastern United States.

This work analyzes PM2.5 24-h average concentrations measured every third day at over 300 locations in the eastern United States during 2000. The non-negative factor analytic model, Positive Matrix Factorization, has been enhanced by modeling the dependence of PM2.5 concentrations on temperature, humidity, pressure, ozone concentrations, and wind velocity vectors. The model comprises 12 general factors, augmented by 5 urban-only factors intended to represent excess concentration present in urban locations only. The computed factor components or concentration fields are displayed as concentration maps, one for each factor, showing how much each factor contributes to the average concentration at each location. The factors are also displayed as flux maps that illustrate the spatial movement of PM2.5 aerosol, thus enabling one to pinpoint potential source areas of PM2.5. The quality of the results was investigated by examining how well the model reproduces especially high concentrations of PM2.5 on specific days at specific locations. Delimiting the spatial extent of all such factors that exhibit a clear regional maximum surrounded by an almost-zero outer domain lowered the uncertainty in the computed results.

Aerosols↗

PubMed2003

Locating and quantifying PCB sources in Chicago: receptor modeling and field sampling.

Potential source contribution function (PSCF) modeling using polychlorinated biphenyl (PCB) concentrations measured in the Chicago area resolved three PCB source sectors. They were (i) the direction northwest of Chicago, (ii) the direction southwest of Chicago, and (iii) the south side of Chicago in the neighborhood of Lake Calumet. The area south of Chicago was further examined by taking upwind/ downwind samples near a landfill and sludge drying beds. Results identified the sludge drying beds and a large landfill as PCB sources to the atmosphere. Another PCB source identified in Chicago was a transformer storage yard. This site had the highest upwind/downwind concentration increments in this study (downwind PCB concentrations were more than 5 times those in the upwind air). These PCB sources were characterized in terms of inventories, emission rates, contributions, and PCB congener profiles (fingerprints). Preliminarily results indicate that the sludge may emit up to 90 kg/yr of PCBs to the air. This amount is probably not a significant contribution of PCBs to the Chicago atmosphere on the basis of dispersion modeling results and a simple box model.

Chicago↗

PubMed2003

Measured summertime concentrations of particulate components, Hg0, and speciated polycyclic aromatic hydrocarbons at rural sites in New York State.

Daily PM2.5 samples, Hg0 and speciated polycyclic aromatic hydrocarbon (PAH) were simultaneously collected at Potsdam and Stockton site in NY during the summers of 2000 and 2001. Samples for determination of the mass concentration and chemical composition of the PM2.5 were obtained with a speciation network PM2.5 sampler. Chemical composition including trace elemental composition, water-soluble ions, and elemental carbon were analyzed. Elemental mercury and PAHs were sampled separately. Daily PM2.5 concentrations ranged from 0.47 to 53.7 microg m(-3) at the Potsdam site, and from 0.82 to 47.23 microg m(-3) at the Stockton site with large daily differences between the two sites. Potsdam consistently had lower mass values than Stockton. The greatest contributors to the PM2.5 mass (generally >0.1 microg/m(3)) were sulfate, nitrate, ammonium, and BC at both sites. Seventeen PAHs were identified at each site in 2000 and the average total concentrations were 3.2 ng/m(3) and 2.9 ng/m(3) at the Potsdam and Stockton sites, respectively. The mean vapor phase mercury concentration at the Potsdam site (2.4 +/-1.2 ng m(-3), n=93) was higher than that at the Stockton site (1.2 +/- 1.0 ng m(-3), n=60) in 2000, whereas in 2001, the average concentrations were 1.1 ng m(-3) and 1.6 ng m(-3) at the Potsdam and Stockton sites, respectively. In general, vapor phase mercury concentrations increased with increasing ambient temperature at the Stockton site in 2000. These differences in values between 2000 and 2001 can be largely explained by distinct differences in the meteorological regimes that dominated in the different years.

Aerosols↗

PubMed2003

Source identification of atlanta aerosol by positive matrix factorization.

Data characterizing daily integrated particulate matter (PM) samples collected at the Jefferson Street monitoring site in Atlanta, GA, were analyzed through the application of a bilinear positive matrix factorization (PMF) model. A total of 662 samples and 26 variables were used for fine particle (particles < or = 2.5 microm in aerodynamic diameter) samples (PM2.5), and 685 samples and 15 variables were used for coarse particle (particles between 2.5 and 10 microm in aerodynamic diameter) samples (PM10-2.5). Measured PM mass concentrations and compositional data were used as independent variables. To obtain the quantitative contributions for each source, the factors were normalized using PMF-apportioned mass concentrations. For fine particle data, eight sources were identified: SO4(2-) -rich secondary aerosol (56%), motor vehicle (22%), wood smoke (11%), NO(3-) -rich secondary aerosol (7%), mixed source of cement kiln and organic carbon (OC) (2%), airborne soil (1%), metal recycling facility (0.5%), and mixed source of bus station and metal processing (0.3%). The SO4(2-) -rich and NO(3-) -rich secondary aerosols were associated with NH(4+). The SO4(2-) -rich secondary aerosols also included OC. For the coarse particle data, five sources contributed to the observed mass: airborne soil (60%), NO(3-)-rich secondary aerosol (16%), SO4(2-) -rich secondary aerosol (12%), cement kiln (11%), and metal recycling facility (1%). Conditional probability functions were computed using surface wind data and identified mass contributions from each source. The results of this analysis agreed well with the locations of known local point sources.

Air Pollutants, Occupational↗

PubMed2002

Identification of sources contributing to Mid-Atlantic regional aerosol.

Source types or source regions contributing to the concentration of atmospheric fine particles measured at Brigantine National Wildlife Refuge, NJ, were identified using a factor analysis model called Positive Matrix Factorization (PMF). Cluster analysis of backward air trajectories on days of high- and low-factor concentrations was used to link factors to potential source regions. Brigantine is a Class I visibility area with few local sources in the center of the eastern urban corridor and is therefore a good location to study Mid-Atlantic regional aerosol. Sulfate (expressed as ammonium sulfate) was the most abundant species, accounting for 49% of annual average fine mass. Organic compounds (22%; expressed as 1.4 x organic carbon) and ammonium nitrate (10%) were the next abundant species. Some evidence herein suggests that secondary organic aerosol formation is an important contributor to summertime regional aerosol. Nine factors were identified that contributed to PM2.5 mass concentrations: coal combustion factors (66%, summer and winter), sea salt factors (9%, fresh and aged), motor vehicle/mixed combustion (8%), diesel/Zn-Pb (6%), incinerator/industrial (5%), oil combustion (4%), and soil (2%). The aged sea salt concentrations were highest in springtime, when the land breeze-sea breeze cycle is strongest. Comparison of backward air trajectories of high- and low-concentration days suggests that Brigantine is surrounded by sources of oil combustion, motor vehicle/mixed combustion, and waste incinerator/industrial emissions that together account for 17% of PM2.5 mass. The diesel/Zn-Pb factor was associated with sources north and west of Brigantine. Coal combustion factors were associated with coal-fired power plants west and southwest of the site. Particulate carbon was associated not only with oil combustion, motor vehicle/mixed combustion, waste incinerator/industrial, and diesel/Pb-Zn, but also with the coal combustion factors, perhaps through common transport.

Aerosols↗