Modeling wintertime particulate matter formation in central California

A wintertime episode during the 2000 California Regional PM Air Quality Study (CRPAQS) was simulated with the air quality model CMAQ–MADRID. Model performance was evaluated with 24-h average measurements available from CRPAQS. Modeled organic matter (OM) was dominated by emissions, which were probably significantly under-represented, especially in urban areas. In one urban area, modeled daytime nitrate concentrations were low and evening concentrations were high. This diurnal profile was not explained by the partition of nitrate between the gas and particle phases, because gaseous nitric acid concentrations were low compared to PM nitrate. Both measured and simulated nitrate concentrations aloft were lower than at the surface at two tower locations during this episode. Heterogeneous reactions involving NO₃ and N₂O₅ accounted for significant nitrate production in the model, resulting in a nighttime peak. The sensitivity of PM nitrate to precursor emissions varied with time and space. Nitrate formation was on average sensitive to NO_x emissions. However, for some periods at urban locations, reductions in NO_x caused the contrary response of nitrate increases. Nitrate was only weakly sensitive to reductions in anthropogenic VOC emissions. Nitrate formation tended to be insensitive to the availability of ammonia at locations with high nitrate, although the spatial extent of the nitrate plume was reduced when ammonia was reduced. Reductions in PM emissions caused OM to decrease, but had no effect on nitrate despite the role of heterogeneous reactions. A control strategy that focuses on NO_x and PM emissions would be effective on average, but reductions in VOC and NH₃ emissions would also be beneficial for certain times and locations.     

光散射颗粒物监测仪在环境空气监测中的适用性

为了研究光散射颗粒物监测仪在环境空气监测中的适应性,参照《环境空气颗粒物(PM10和PM2.5)连续自动检测技术要求及检测方法》(HJ 653-2013),在北京秋季使用PQ200(滤膜采样器)对DustTrak8530、LD-6S、HBKLW-2共3种光散射仪器进行比对测试.结果表明,3种光散射仪器的平行性都达标;在监测PM10时,3种仪器与PQ200的线性相关系数都达标,斜率只有HBKLW-2达标,截距除HBKLW-2略微超标外都与标准相差较远;在监测PM2.5时,3种仪器与PQ200的线性相关系数都达标且优于PM10,斜率只有HBKLW-2和LD-6S达标,截距绝对值相比PM10有所减小,但只有HBKLW-2达标;经校正因子修正后,3种仪器与PQ200的线性回归斜率达标、相关系数不变、监测PM2.5的截距相比PM10更加接近标准值,故光散射仪器更加适用于环境空气PM2.5监测.     

Dicarboxylic acids and related compounds in fine particulate matter aerosols in Huangshi,central China

PM_2.5 (particulate matter with an aerodynamic diameter <2.5 μm) samples were collected in Huangshi, central China, from March 2012 to February 2013 and were analyzed for dicarboxylic acids (diacids) and related compounds (DARCs). Oxalic acid (C₂; 416 ng m^?3) was the most abundant species, followed by phthalic (Ph; 122 ng m^?3), terephthalic (tPh; 116 ng m^?3), succinic (C₄; 70.4 ng m^?3), azelaic (C₉; 67.9 ng m^?3), and adipic (C₆; 57.8 ng m^?3) acids. Relatively high abundances of Ph and tPh differed from the distribution in urban and marine aerosols, indicating contributions from nearby anthropogenic sources. Glyoxylic acid (ωC₂; 41.4 ng m^?3) was the dominant oxoacid, followed by 9-oxononanoic (ωC₉; 40.8 ng m^?3) and pyruvic (Pyr; 24.1 ng m^?3) acids. Glyoxal (Gly; 35.5 ng m^?3) was the dominant α-dicarbonyl. Highest average concentrations were found for C₂, ωC₂, and C₉ in autumn, for C₄, for Pyr and C₆ in spring, for Ph, ωC₉, and Gly in summer, whereas the lowest values were observed in winter. Seasonal variations and correlation coefficients of DARCs demonstrate that both primary emissions and secondary production are important sources. Principal component analysis of selected DARCs species suggests that a mixing of air masses from anthropogenic and biogenic sources contribute to the Huangshi aerosols.

Implications: Both primary emissions and secondary production are important sources of diacids and related compounds in PM_2.5 from Huangshi, central China. Principal component analysis of selected diacids in Huangshi aerosols suggests that mixing of air masses from anthropogenic and biogenic sources contribute to ambient aerosols in central China.     

Regional contributions to airborne particulate matter in central California during a severe pollution episode

The externally-mixed source-oriented UCD/CIT air quality model was applied to determine the significance of inter-regional transport for primary and secondary particulate matter (PM) in California's Central Valley during a severe wintertime PM pollution episode from December 15, 2000 to January 7, 2001. The gases and primary PM emitted from eight different geographical sub-regions were tracked separately in a model simulation that included transport, physical and chemical transformation and deposition processes. The model results directly predict the contribution that each sub-region makes to PM concentrations throughout the entire model domain. The boundary layer was relatively stagnant during the simulated 3-week air quality episode, and no consistent transport pattern for primary PM was predicted. Several significant inter-regional transport events were identified that each lasted a few days. Each of these inter-regional events was characterized by transport of gas-phase precursors of nitrate that combined with local emissions of ammonia to produce particulate nitrate. Nitrate already in the particle phase was not transported efficiently due to higher dry deposition rates for particles relative to gas-phase nitrogen oxides. The distinctive pattern of transport for nitrate precursors reflects the relatively long timescales required to convert NO_x emissions to nitrate during winter conditions characterized by low temperatures, weak photolysis rates, and low oxidant concentrations. The equilibrium partitioning of nitrate and ammonia to the particle phase is relatively fast once the nitrate has been produced. The most-likely transport distance for nitrate during the current episode varied from 130–140 km for the northern portion of the Central Valley to 50–60 km in the southern portion of the Central Valley. Sub-regions further south in the Valley have smaller transport distances because of slower wind speeds and the greater abundance of ammonia in these areas, leading to faster conversion of gas-phase reactive nitrogen into particulate nitrate, which has a higher dry deposition rate than the gas-phase species. The most-likely transport distance for primary organic compounds (OC) was found to be less than that for nitrate, varying from 50 to 60 km for the northern portion of the Valley to 20–30 km for southern portion of the Valley. Overall, 68% of the particulate nitrate formed in the most polluted sub-regions of the Central Valley originates from emissions in those same sub-regions. Local emissions controls should therefore provide an effective strategy to reduce airborne particulate matter concentrations to acceptable levels.     

Determination of levoglucosan in atmospheric fine particulate matter

A microanalytical method suitable for the quantitative determination of the sugar anhydride levoglucosan in low-volume samples of atmospheric fine particulate matter (PM) has been developed and validated. The method incorporates two sugar anhydrides as quality control standards. The recovery standard sedoheptulosan (2,7-anhydro-beta-D-altro-heptulopyranose) in 20 microL solvent is added onto samples of the atmospheric fine PM and aged for 1 hr before ultrasonic extraction with ethylacetate/ triethylamine. The extract is reduced in volume, an internal standard is added (1,5-anhydro-D-mannitol), and a portion of the extract is derivatized with 10% by volume N-trimethylsilylimidazole. The derivatized extract is analyzed by gas chromatography/mass spectrometry (GC/MS). The recovery of levoglucosan using this procedure was 69 +/- 6% from five filters amended with 2 microg levoglucosan, and the reproducibility of the assay is 9%. The limit of detection is approximately 0.1 microg/mL, which is equivalent to approximately 3.5 ng/m3 for a 10 L/min sampler or approximately 8.7 ng/m3 for a 4 L/min personal sampler (assuming 24-hr integrated samples). We demonstrated that levoglucosan concentrations in collocated samples (expressed as ng/m3) were identical irrespective of whether samples were collected by PM with aerodynamic diameter < or = 2.5 microm or PM with aerodynamic diameter < or = 10 microm impactors. It was also demonstrated that X-ray fluorescence analysis of samples of atmospheric PM, before levoglucosan determinations, did not alter the levels of levoglucosan.     

Personal exposure to fine particulate matter concentrations in central business district of a tropical coastal city

In the present study, personal exposure to fine particulate matter (particulate matter with an aerodynamic diameter <2.5 μm [PM_2.5]) concentrations in an urban hotspot (central business district [CBD]) was investigated. The PM monitoring campaigns were carried out at an urban hotspot from June to October 2015. The personal exposure monitoring was performed during three different time periods, i.e., morning (8 a.m.?9 a.m.), afternoon (12.30 p.m.–1.30 p.m.), and evening (4 p.m.–5 p.m.), to cover both the peak and lean hour activities of the CBD. The median PM_2.5 concentrations were 38.1, 34.9, and 40.4 µg/m³ during the morning, afternoon, and evening hours on the weekends. During weekdays, the median PM_2.5 concentrations were 59.5, 29.6, and 36.6 µg/m³ in the morning, afternoon, and evening hours, respectively. It was observed that the combined effect of traffic emissions, complex land use, and micrometeorological conditions created localized air pollution hotspots. Furthermore, the total PM_2.5 lung dose levels for an exposure duration of 1 hr were 8.7 ± 5.7 and 12.3 ± 5.2 µg at CBD during weekends and weekdays, respectively, as compared with 2.5 ± 0.8 µg at the urban background (UB). This study emphasizes the need for mobile measurement for short-term personal exposure assessment complementing the fixed air quality monitoring.

Implications: Personal exposure monitoring at an urban hotspot indicated space and time variation in PM concentrations that is not captured by the fixed air quality monitoring networks. The short-term exposure to higher concentrations can have a significant impact on health that need to be considered for the health risk–based air quality management. The study emphasizes the need of hotspot-based monitoring complementing the already existing fixed air quality monitoring in urban areas. The personal exposure patterns at hotspots can provide additional insight into sustainable urban planning.     

Oxalic acid in PM2.5 particulate matter in California

Ambient air monitoring for organic acids in PM2.5 was conducted at several locations in California. During the study, it was found that oxalic acid (ethanedioc acid) was the most abundant organic acid found in the PM2.5 fraction. Samples from Azuza (in southern California), San Jose (in the San Francisco Bay area), and Fresno (in central California), a PM2.5 Super Site, were collected in 1999 and analyzed. The results for oxalic acid concentrations during this monitoring effort are presented.     

Spatial and temporal variability in urban fine particulate matter concentrations

Identification of hot spots for urban fine particulate matter (PM(2.5)) concentrations is complicated by the significant contributions from regional atmospheric transport and the dependence of spatial and temporal variability on averaging time. We focus on PM(2.5) patterns in New York City, which includes significant local sources, street canyons, and upwind contributions to concentrations. A literature synthesis demonstrates that long-term (e.g., one-year) average PM(2.5) concentrations at a small number of widely-distributed monitoring sites would not show substantial variability, whereas short-term (e.g., 1-h) average measurements with high spatial density would show significant variability. Statistical analyses of ambient monitoring data as a function of wind speed and direction reinforce the significance of regional transport but show evidence of local contributions. We conclude that current monitor siting may not adequately capture PM(2.5) variability in an urban area, especially in a mega-city, reinforcing the necessity of dispersion modeling and methods for analyzing high-resolution monitoring observations.     

Transport of atmospheric fine particulate matter: part 2--findings from recent field programs on the intraurban variability in fine particulate matter

Air quality field data, collected as part of the fine particulate matter Supersites Program and other field measurements programs, have been used to assess the degree of intraurban variability for various physical and chemical properties of ambient fine particulate matter. Spatial patterns vary from nearly homogeneous to quite heterogeneous, depending on the city, parameter of interest, and the approach or method used to define spatial variability. Secondary formation, which is often regional in nature, drives fine particulate matter mass and the relevant chemical components toward high intraurban spatial homogeneity. Those particulate matter components that are dominated by primary emissions within the urban area, such as black carbon and several trace elements, tend to exhibit greater spatial heterogeneity. A variety of study designs and data analysis approaches have been used to characterize intraurban variability. High temporal correlation does not imply spatial homogeneity. For example, there can be high temporal correlation but with spatial heterogeneity manifested as smooth spatial gradients, often emanating from areas of high emissions such as the urban core or industrial zones.     

Feasibility of using low-cost portable particle monitors for measurement of fine and coarse particulate matter in urban ambient air

Exposure to ambient particulate matter (PM) is known as a significant risk factor for mortality and morbidity due to cardiorespiratory causes. Owing to increased interest in assessing personal and community exposures to PM, we evaluated the feasibility of employing a low-cost portable direct-reading instrument for measurement of ambient air PM exposure. A Dylos DC 1700 PM sensor was collocated with a Grimm 11-R in an urban residential area of Houston Texas. The 1-min averages of particle number concentrations for sizes between 0.5 and 2.5 µm (small size) and sizes larger than 2.5 µm (large size) from a DC 1700 were compared with the 1-min averages of PM_2.5 (aerodynamic size less than 2.5 µm) and coarse PM (aerodynamic size between 2.5 and 10 µm) concentrations from a Grimm 11-R. We used a linear regression equation to convert DC 1700 number concentrations to mass concentrations, utilizing measurements from the Grimm 11-R. The estimated average DC 1700 PM_2.5 concentration (13.2 ± 13.7 µg/m³) was similar to the average measured Grimm 11-R PM_2.5 concentration (11.3 ± 15.1 µg/m³). The overall correlation (r²) for PM_2.5 between the DC 1700 and Grimm 11-R was 0.778. The estimated average coarse PM concentration from the DC 1700 (5.6 ± 12.1 µg/m³) was also similar to that measured with the Grimm 11-R (4.8 ± 16.5 µg/m³) with an r² of 0.481. The effects of relative humidity and particle size on the association between the DC 1700 and the Grimm 11-R results were also examined. The calculated PM mass concentrations from the DC 1700 were close to those measured with the Grimm 11-R when relative humidity was less than 60% for both PM_2.5 and coarse PM. Particle size distribution was more important for the association of coarse PM between the DC 1700 and Grimm 11-R than it was for PM_2.5.

Implications: The performance of a low-cost particulate matter (PM) sensor was evaluated in an urban residential area. Both PM_2.5 and coarse PM (PM_10-2.5) mass concentrations were estimated using a DC1700 PM sensor. The calculated PM mass concentrations from the number concentrations of DC 1700 were close to those measured with the Grimm 11-R when relative humidity was less than 60% for both PM_2.5 and coarse PM. Particle size distribution was more important for the association of coarse PM between the DC 1700 and Grimm 11-R than it was for PM_2.5.     

Sources of fine urban particulate matter in Detroit, MI

Data from the speciation trends network (STN) was used to evaluate the amount and temporal patterns of particulate matter originating from local industrial sources and long-range transport at two sites in Detroit, MI: Allen Park, MI, southwest of both Detroit and the areas of heavy industrial activity; Dearborn, MI, located on the south side of Detroit near the most heavily industrialized region. Using positive matrix factorization (PMF) and comparing source contributions at Allen Park to those in Dearborn, contributions made by local industrial sources (power plants, coke refineries, iron smelting, waste incineration), local area sources (automobile and diesel truck) and long range sources of PM(2.5) can be distinguished in greater Detroit. Overall, the mean mass concentration measured at Dearborn was 19% higher than that measured at Allen Park. The mass at Allen Park was apportioned as: secondary sulfate 31%, secondary nitrate 28%, soil 8%, mixed aged sea and road salts 4%, gasoline 15%, diesel 4%, and biomass burning 3%. At Dearborn the mass was apportioned as: secondary sulfate 25%, secondary nitrate 20%, soil 12%, mixed aged sea and road salts 4%, gasoline 20%, diesel 8%, iron and steel, 5%, and mixed industrial 7%. The impact of the iron and steel, soil, and mixed aged sea and road salt was much higher at the Dearborn site than at the Allen Park site, suggesting that close proximity to a local industrial complex has a direct negative impact on local air quality.     

Source contributions to fine particulate matter in an urban atmosphere

This paper proposes a practical method for estimating source attribution by using a three-step methodology. The main objective of this study is to explore the use of the three-step methodology for quantifying the source impacts of 24-h PM2.5 particles at an urban site in Seoul, Korea. 12-h PM2.5 samples were collected and analyzed for their elemental composition by ICP-AES/ICP-MS/AAS to generate the source composition profiles. In order to assess the daily average PM2.5 source impacts, 24-h PM2.5 and polycyclic aromatic hydrocarbons (PAH) ambient samples were simultaneously collected at the same site. The PM2.5 particle samples were then analyzed for trace elements. Ionic and carbonaceous species concentrations were measured by ICP-AES/ICP-MS/AAS, IC, and a selective thermal MnO2 oxidation method. The 12-h PM2.5 chemical data was used to estimate possible source signatures using the principal component analysis (PCA) and the absolute principal component scores method followed by the multiple linear regression analysis. The 24-h PM2.5 source categories were extracted with a combination of PM2.5 and some PAH chemical data using the PCA, and their quantitative source contributions were estimated by chemical mass balance (CMB) receptor model using the estimated source profiles and those in the literature. The results of PM2.5 source apportionment using the 12-h derived source composition profiles show that the CMB performance indices; chi2, R2, and percent of mass accounted for are 2.3%, 0.97%, and 100.7%, which are within the target range specified. According to the average PM2.5 source contribution estimate results, motor vehicle exhaust was the major contributor at the sampling site, contributing 26% on average of measured PM2.5 mass (41.8 microg m-3), followed by secondary sulfate (23%) and nitrate (16%), refuse incineration (15%), soil dust (13%), field burning (4%), oil combustion (2.7%), and marine aerosol (1.3%). It can be concluded that quantitative source attribution to PM2.5 in an urban area where source profiles have not been developed can be estimated using the proposed three-step methodology approach.     

人体室内外PM_(2.5)吸入暴露研究

介绍了室内外空气颗粒物吸入暴露的评价方法,选择PM2.5作为检测评价的对象,初步评价了上海市某区不同年龄段人员的PM2.5暴露水平。结果表明:(1)成人和老人的全年日平均PM2.5吸入暴露量均较高,并且成人的全年日平均PM2.5吸入暴露量变化曲线和儿童相似。(2)老人室内PM2.5吸入暴露量要明显高于室外,其主要原因是老人在室内时间较长。儿童和成人的室外PM2.5吸入暴露量高于室内。(3)不同人员的年平均PM2.5吸入暴露量的排序为成人老人儿童,其年平均PM2.5吸入暴露量分别为1.141、1.046、0.935mg。     

Trends in fine particle concentration and chemical composition in southern California

Airborne fine particle mass concentrations in Southern California have declined in recent years. Trends in sulfate and elemental carbon (EC) particle concentrations over the period 1982-1993 are consistent with this overall improvement in air quality and help to confirm some of the reasons for the changes that are seen. Fine particle sulfate concentrations have declined as a strict sulfur oxides (SOx) emission control program adopted in 1978 was implemented over time. Fine particle elemental (black) carbon concentrations have declined over a period when newer diesel engines and improved diesel fuels have been introduced into the vehicle fleet. Organic aerosol concentrations have not declined as rapidly as the EC particle concentrations, despite the fact that catalyst-equipped cars having lower particle emission rates were introduced into the vehicle fleet alongside the diesel engine improvements mentioned above. This situation is consistent with the growth in population and vehicle miles traveled in the air basin over time. Fine particle ammonium nitrate in the Los Angeles area atmosphere contributes more than half of the fine aerosol mass concentration on the highest concentration days of the year, emphasizing both the need for accurate aerosol nitrate measurements and the likely importance of deliberate control of aerosol nitrate as a part of any serious further fine particle control program for the Los Angeles area.     

Comparison of source apportionments of fine particulate matter at two San Jose speciation trends network sites

In this study, the chemical composition of fine particulate matter samples collected at U.S. Environmental Protection Agency Speciation Trends Network sites in San Jose, CA, from February 2000 to February 2005 were analyzed. A San Jose site was initially established at 4th Street and then subsequently moved to Jackson Street in mid-2002. These sites are approximately 1 km apart. There were no known major changes in the nature of the sources in the area over this period. The study used positive matrix factorization model to extract the source profiles and their mass contributions and to compare the results for the congruence of the source apportionments between these two nearby sites. In the case of the 4th Street site, the average mass was apportioned to wood combustion (32.1 +/- 2.5%), secondary nitrate (22.3 +/- 2%), secondary sulfate (10.7 +/- 0.6%), fresh sea salt (7.7 +/- 0.9%), gasoline vehicles (7.3 +/- 0.5%), aged sea salt (6.8 +/- 0.4%), road dust (6.7 +/- 0.7%), diesel emissions (3.9 +/- 0.3%), and a Ni-related industrial source (2.5 +/- 0.4%). At the Jackson Street site, the average mass was apportioned to wood combustion (33.6 +/- 2.6%), secondary nitrate (20.3 +/- 1.9%), secondary sulfate (13.9 +/- 0.9%), aged sea salt (12.4 +/- 0.7%), gasoline vehicle (8.3 +/- 0.6%), fresh sea salt (5.3 +/- 0.5%), diesel emission (3.2 +/- 0.3%), road dust (1.9 +/- 0.1%), and Ni-related industrial source (1.3 +/- 0.1%). Conditional probability function analysis was used to help identify local sources. These results suggested that moving the sampling site a short distance had little effect on the nature of the resolved source types although some differences in their quantitative impacts were obtained in the positive matrix factorization analyses.     

Source apportionment of airborne fine particulate matter in an underground mine

The chemical mass balance source apportionment technique was applied to an underground gold mine to assess the contribution of diesel exhaust, rock dust, oil mists, and cigarette smoke to airborne fine (<2.5 microm) particulate matter (PM). Apportionments were conducted in two locations in the mine, one near the mining operations and one near the exit of the mine where the ventilated mine air was exhausted. Results showed that diesel exhaust contributed 78-98% of the fine particulate mass and greater than 90% of the fine particle carbon, with rock dust making up the remainder. Oil mists and cigarette smoke contributions were below detection limits for this study. The diesel exhaust fraction of the total fine PM was higher than the recently implemented mine air quality standards based on total carbon at both sample locations in the mine.     

Characterization of visibility impacts related to fine particulate matter in Canada

Canada has recently established standards for the management of particulate matter (PM) air quality. National networks currently measure PM mass concentrations and chemical speciation. Methods used in the U.S. IMPROVE network are applied to the 1994--2000 Canadian fine PM data to obtain a regional reconstruction of the visibility based on particle composition. Nationally, the greatest light extinction occurs in the Windsor-Quebec City corridor. Variations in the dominant chemical species responsible for the reduction in visibility are presented for regions across the country. In most regions, sulfate and nitrate contribute most greatly to reduced visibility. The visibility implications of achieving the Canada-Wide Standard (CWS) across the country are evaluated, with the greatest improvement in visibility associated with achieving the CWS in southern Ontario. Elsewhere in the country, achieving the CWS will actually result in deteriorating air quality. Improving current estimates of visibility requires higher spatially and temporally resolved measurements of organic and elemental carbon fractions and particulate nitrate.     

Size and composition distribution of airborne particulate matter in northern California: I--particulate mass, carbon, and water-soluble ions

The San Joaquin Valley (SJV) in California has one of the most severe particulate air quality problems in the United States during the winter season. In the current study, measurements of particulate matter (PM) smaller than 10 microm in aerodynamic diameter (PM10), fine particles (PM18), and ultrafine particles (PM0.1) made during the period December 16, 2000-February 3, 2001, at six locations near or within the SJV are discussed: Bodega Bay, Davis, Sacramento, Modesto, Bakersfield, and Sequoia National Park. Airborne PM1.8 concentrations at the most heavily polluted site (Bakersfield) increased from 20 to 172 microg/m3 during the period December 16, 2000-January 7, 2001. The majority of the fine particle mass was ammonium nitrate driven by an excess of gas-phase ammonia. Peak PM0.1 concentrations (8-12 hr average) were approximately 2.4 microg/m3 measured at night in Sacramento and Bakersfield. Ultrafine particle concentrations were distinctly diurnal, with daytime concentrations approximately 50% lower than nighttime concentrations. PMO.1 concentrations did not accumulate during the multiweek stagnation period; rather, PMO.1 mass decreased at Bakersfield as PM1.8 mass was increasing. The majority of the ultrafine particle mass was associated with carbonaceous material. The high concentrations of ultrafine particles in the SJV pose a potential serious public health threat that should be addressed.