Characterization of Carbonaceous Species of Ambient PM2.5 in Beijing,China

Abstract

One-week integrated fine particulate matter (i.e., particles <2.5 μm in diameter; PM_2.5) samples were collected continuously with a low-flow rate sampler at a downtown site (Chegongzhuang) and a residential site (Tsinghua University) in Beijing between July 1999 and June 2000. The annual average concentrations of organic carbon (OC) and elemental carbon (EC) at the urban site were 23.9 and 8.8 μg m^?3, much higher than those in some cities with serious air pollution. Similar weekly variations of OC and EC concentrations were found for the two sampling sites with higher concentrations in the winter and autumn. The highest weekly variations of OC and EC occurred in the winter, suggesting that combustion sources for space heating were important contributors to carbonaceous particles, along with a significant impact from variable meteorological conditions. High emissions coupled with unfavorable meteorological conditions led to the max weekly carbonaceous concentration the week of November 18–25, 1999. The weekly mass ratios of OC:EC ranged between 2 and 4 for most samples and averaged 2.9, probably suggesting that secondary OC (SOC) is present most weeks. The range of contemporary carbon fraction, based on the C14 analyses of eight samples collected in 2001, is 0.330–0.479. Estimated SOC accounted for ～38% of the total OC at the two sites. Average OC and EC concentrations at Tsinghua University were 25% and 18%, respectively, higher than those at Chegongzhuang, which could be attributed to different local emissions of primary carbonaceous particles and gaseous precursors of SOC, as well as different summer photochemical intensities between the two locations.     

Method Comparisons for Particulate Nitrate,Elemental Carbon,and PM2.5 Mass in Seven U.S. Cities

ABSTRACT

Methods that measure PM₂₅ mass, total particulate NO₃ ^-, and elemental carbon (EC) were evaluated in seven U.S. cities from 1997 to 1999. Sampling was performed in Bakersfield, CA; Boston, MA; Chicago, IL; Dallas, TX; Philadelphia, PA; Phoenix, AZ; and Riverside, CA. Evaluating and validating methods that measure the components of fine mass are important to the effort of establishing a speciation-monitoring network. The Harvard Impactor (HI), which measures fine particle mass, showed excellent agreement (r² = 0.99) with the PM₂₅ Federal Reference Method (FRM) for 81 24-hr samples in Riverside and Bakersfield. The HI also showed good precision (4.8%) for 243 24-hr collocated samples over eight studies.

The Aethalometer was employed in six of the sampling locations to measure black carbon (BC). These values were compared to EC as measured from a quartz filter using thermal analysis. For the six cities combined, the two methods were highly correlated (r² = 0.94; 187 24-hr samples); however, the BC values were approximately 24% less than the EC measurements consistently across all six cites. This compares well to results observed for EC/BC measurements observed in other semi-urban areas. Par-ticulate NO₃ ^- was measured using the Harvard-EPA Annular Denuder System (HEADS). This was compared to the NO₃ ^- measured from the HI Teflon (DuPont) filter to assess NO₃ ^- artifacts. Significant NO₃ ^- losses (approximately 50% of total NO₃ ^-) were found in Riverside, Philadelphia, and Boston, while minimal artifacts were observed in the other sites. Two types of HEADS configurations were employed in five cities. One system used a Na₂CO₃-coated glass fiber filter, and the other type used a nylon filter to collect volatilized NO₃ ^- from the Teflon filter. The HEADS with the Na₂CO₃-coated filter consistently underestimated the total particulate NO₃ ^- by approximately 20% compared to the nylon HEADS.     

Loss of PM2.5 Nitrate from Filter Samples in Central California

Abstract

Evaporative loss of particulate matter (with aerodynamic diameter <2.5 μm, [PM_2.5]) ammonium nitrate from quartz-fiber filters during aerosol sampling was evaluated from December 3, 1999, through February 3, 2001, at two urban (Fresno and Bakersfield) and three nonurban (Bethel Island, Sierra Nevada Foothills, and Angiola) sites in central California. Compared with total particulate nitrate, evaporative nitrate losses ranged from <10% during cold months to >80% during warm months. In agreement with theory, evaporative loss from quartz-fiber filters in nitric acid denuded samplers is controlled by the ambient nitric acid-to-particulate nitrate ratio, which is determined mainly by ambient temperature. Accurate estimation of nitrate volatilization requires a detailed thermodynamic model and comprehensive chemical measurements. For the 14-month average of PM_2.5 acquired on Teflon-membrane filters, measured PM_2.5 mass was 8–16% lower than actual PM_2.5 mass owing to nitrate volatilization. For 24-hr samples, measured PM_2.5 was as much as 32–44% lower than actual PM_2.5 at three California Central Valley locations.     

Contribution of primary and secondary sources to organic aerosol and PM2.5 at SEARCH network sites

Chemical tracer methods for determining contributions to primary organic aerosol (POA) are fairly well established, whereas similar techniques for secondary organic aerosol (SOA), inherently complicated by time-dependent atmospheric processes, are only beginning to be studied. Laboratory chamber experiments provide insights into the precursors of SOA, but field data must be used to test the approaches. This study investigates primary and secondary sources of organic carbon (OC) and determines their mass contribution to particulate matter 2.5 microm or less in aerodynamic diameter (PM2.5) in Southeastern Aerosol Research and Characterization (SEARCH) network samples. Filter samples were taken during 20 24-hr periods between May and August 2005 at SEARCH sites in Atlanta, GA (JST); Birmingham, AL (BHM); Centerville, AL (CTR); and Pensacola, FL (PNS) and analyzed for organic tracers by gas chromatography-mass spectrometry. Contribution to primary OC was made using a chemical mass balance method and to secondary OC using a mass fraction method. Aerosol masses were reconstructed from the contributions of POA, SOA, elemental carbon, inorganic ions (sulfate [SO4(2-)], nitrate [NO3-], ammonium [NH4+]), metals, and metal oxides and compared with the measured PM2.5. From the analysis, OC contributions from seven primary sources and four secondary sources were determined. The major primary sources of carbon were from wood combustion, diesel and gasoline exhaust, and meat cooking; major secondary sources were from isoprene and monoterpenes with minor contributions from toluene and beta-caryophyllene SOA. Mass concentrations at the four sites were determined using source-specific organic mass (OM)-to-OC ratios and gave values in the range of 12-42 microg m(-3). Reconstructed masses at three of the sites (JST, CTR, PNS) ranged from 87 to 91% of the measured PM2.5 mass. The reconstructed mass at the BHM site exceeded the measured mass by approximately 25%. The difference between the reconstructed and measured PM2.5 mass for nonindustrial areas is consistent with not including aerosol liquid water or other sources of organic aerosol.     

Contribution of Primary and Secondary Sources to Organic Aerosol and PM2.5 at SEARCH Network Sites

Abstract

Chemical tracer methods for determining contributions to primary organic aerosol (POA) are fairly well established, whereas similar techniques for secondary organic aerosol (SOA), inherently complicated by time-dependent atmospheric processes, are only beginning to be studied. Laboratory chamber experiments provide insights into the precursors of SOA, but field data must be used to test the approaches. This study investigates primary and secondary sources of organic carbon (OC) and determines their mass contribution to particulate matter 2.5 µm or less in aerodynamic diameter (PM_2.5) in Southeastern Aerosol Research and Characterization (SEARCH) network samples. Filter samples were taken during 20 24-hr periods between May and August 2005 at SEARCH sites in Atlanta, GA (JST); Birmingham, AL (BHM); Centerville, AL (CTR); and Pensacola, FL (PNS) and analyzed for organic tracers by gas chromatography-mass spectrometry. Contribution to primary OC was made using a chemical mass balance method and to secondary OC using a mass fraction method. Aerosol masses were reconstructed from the contributions of POA, SOA, elemental carbon, inorganic ions (sulfate [SO₄ ^2?], nitrate [NO₃ ^?], ammonium [NH₄ ⁺]), metals, and metal oxides and compared with the measured PM_2.5. From the analysis, OC contributions from seven primary sources and four secondary sources were determined. The major primary sources of carbon were from wood combustion, diesel and gasoline exhaust, and meat cooking; major secondary sources were from isoprene and monoterpenes with minor contributions from toluene and β-caryophyllene SOA. Mass concentrations at the four sites were determined using source-specific organic mass (OM)-to-OC ratios and gave values in the range of 12–42 µg m^?3. Reconstructed masses at three of the sites (JST, CTR, PNS) ranged from 87 to 91% of the measured PM_2.5 mass. The reconstructed mass at the BHM site exceeded the measured mass by approximately 25%. The difference between the reconstructed and measured PM_2.5 mass for nonindustrial areas is consistent with not including aerosol liquid water or other sources of organic aerosol.     

Modifications to the Sunset Laboratory Carbon Aerosol Monitor for the Simultaneous Measurement of PM2.5 Nonvolatile and Semi-Volatile Carbonaceous Material

Abstract

Semi-volatile organic carbonaceous material (SVOC) in fine particles is not reliably measured with conventional semicontinuous carbon monitors because semi-volatile carbonaceous material is lost from the collection media during sample collection. Two modifications of a Sunset Laboratory carbon aerosol monitor allowing for the determination of semi-volatile fine particulate organic material are described. Collocated conventional and modified instruments were operated simultaneously using a common inlet. Comparisons were made with integrated PC-BOSS data for quartz filter retained nonvolatile organic carbon (NVOC) and elemental carbon (EC), SVOC, and total carbon (TC = SVOC + NVOC + EC) and good agreement was observed between TC concentrations during studies conducted in Rubidoux, CA. Precision of the comparison was σ=±1.5 μg-C/m³ (±8%). On the basis of experiments performed with the modified Sunset monitor, a dual-oven Sunset monitor was developed and extensively tested in Lindon, UT; Riverside, CA; and in environmental exposure chambers. The precision for the measurement of TC with the dual-oven instrument was σ = ±1.4 μg-C/m³ (±13%).     

关于PM2.5的综述

综述了大气PM25的来源,样品采集分析,化学组成,病毒机理,对人类健康和大气能见度的影响,以及国内外的研究进展.     

The contribution of PM2.5 to cardiovascular disease in China

Environmental Science and Pollution Research - China is experiencing rapid urbanization and industrialization with correspondingly high levels of air pollution. Although the harm of PM2.5 has been...     

Determination of PM2.5 Sulfate and Nitrate with a PC-BOSS Designed for Routine Sampling for Semi-Volatile Particulate Matter

ABSTRACT

Ambient particles contain substantial quantities of material that can be lost from the particles during sample collection on a filter. These include ammonium nitrate and semi-volatile organic compounds. As a result, the concentrations of these species are often significantly in error for results obtained with a filter pack sampler. The accurate measurement of these semi-volatile fine particulate species is essential for a complete understanding of the possible causes of health effects associated with exposure to fine particles. Past organic compound diffusion denuder samplers developed by the authors (e.g., the Brigham Young University Organic Sampling System [BOSS]) are not amenable to routine field use because of the need to independently determine the gas-phase semi-volatile organic material efficiency of the denuder for each sample. This problem has been eliminated using a combined virtual impactor, particle-concentrator inlet to provide a concentrated stream of 0.1-2.5-μm particles. This is followed by a BOSS diffusion denuder and filter packs to collect particles, including any semi-volatile species lost from the particles during sampling. The samp ler (Particle Concentrator-Brigham Young University Organic Sampling System [PC-BOSS]) contains a post-denuder multifilter pack unit to allow for the routine collection of several sequential samples. The PC-BOSS can be used for the determination of both fine particulate nitrate and semi-volatile organic material without significant “positive” or “negative” sampling artifacts. Validation of the sampler for the determination of PM_2.5 sulfate and nitrate based on comparison of results obtained at Riverside, CA with collocated PC-BOSS, annular denuder, and Chem Spec samplers indicates the PC-BOSS gives accurate results for these species with a precision of ±5-8%. An average of 33% of the PM_2.5 nitrate was lost from the particles during sampling for both denuder and single filter samplers.     

Windblown dust contributes to high PM2.5 concentrations

The revised National Ambient Air Quality Standards for PM include fine particulate standards based upon mass measurements of PM2.5. It is possible in arid and semi-arid regions to observe significant coarse mode intrusion in the PM2.5 measurement. In this work, continuous PM10, PM2.5, and PM1.0 were measured during several windblown dust events in Spokane, WA. PM2.5 constituted approximately 30% of the PM10 during the dust event days, compared with approximately 48% on the non-dusty days preceding the dust events. Both PM10 and PM2.5 were enhanced during the dust events. However, PM1.0 was not enhanced during dust storms that originated within the state of Washington. During a dust storm that originated in Asia and impacted Spokane, PM1.0 was also enhanced, although the Asian dust reached Washington during a period of stagnation and poor dispersion, so that local sources were also contributing to high particulate levels. The "intermodal" region of PM, defined as particles ranging in aerodynamic size from 1.0 to 2.5 microns, was found to represent a significant fraction of PM2.5 (approximately 51%) during windblown dust events, compared with 28% during the non-dusty days before the dust events.     

Semi-volatile species in PM2.5: comparison of integrated and continuous samplers for PM2.5 research or monitoring

Fine particles in urban atmospheres contain substantial quantities of semi-volatile material [e.g., NH4NO3 and semi-volatile organic compounds (SVOCs)] that are lost from particles during collection on a filter. Several diffusion denuder samplers have been developed for the determination of both NO3- and organic semi-volatile fine particulate components. The combination of technology used in the BOSS diffusion denuder sampler and the Harvard particle concentrator has resulted in the Particle Concentrator-Brigham Young University Organic Sampling System (PC-BOSS) for the 24-hr (or less) integrated collection of PM2.5, including NH4NO3 and semi-volatile organic material. Modification of the BOSS sampler allows for the weekly determination of these same species. Combination of BOSS denuder and tapered element oscillating microbalance (TEOM) monitor technology has resulted in the real-time ambient mass sampler (RAMS) for the continuous measurement of PM2.5, including the semi-volatile components. Comparison of the results obtained with the BOSS and with each of the newly developed modifications of the BOSS indicates that the modified versions can be used for the continuous, daily, or weekly monitoring of PM2.5, including semi-volatile species, as appropriate to the design of each sampler.     

Particulate matter in California: part 1--Intercomparison of several PM2.5, PM10-2.5, and PM10 monitoring networks

It will be many years before the recently deployed network of fine particulate matter with an aerodynamic diameter less than 2.5 microm (PM2.5) Federal Reference Method (FRM) samplers produces information on nonattainment areas, trends, and source impacts. However, data on PM2.5 and its major constituents have been routinely collected in California for the past 20 years. The California Air Resources Board operated as many as 20 dichotomous (dichot) samplers for PM2.5 and coarse PM (PM10-2.5). The California Acid Deposition Monitoring Program (CADMP) collected 12-h-average PM2.5 and PM10 from 1988 to 1995 at ten urban and rural sites and 24-h-average PM2.5 at five urban sites since 1995. Beginning in 1994, the Children's Health Study collected 2-week averages of PM2.5 in 12 communities in southern California using the Two-Week Sampler (TWS). Comparisons of collocated samples establish relationships between the dichot, CADMP, and TWS samplers and the 82-site network of PM2.5 FRM samplers deployed since 1999 in California. PM mass data from the different monitoring programs have modest to high correlation to FRM mass data, fairly small systematic biases and negative proportional biases ranging from 7 to 22%. If the biases are taken into account, all of the programs should be considered comparable with the FRM program. Thus, historical data can be used to develop long-term PM trends in California.     

贵阳市白云区大气PM_(10)和PM_(2.5)污染特征

使用β射线法在线监测仪连续监测了贵阳市白云区PM_(10)和PM_(2.5)浓度,分析了2014年6月1日—12月31日7个月内PM_(10)、PM_(2.5)的浓度水平、时变规律和PM_(2.5)/PM_(10)的变化情况。结果表明,监测时段内PM_(10)和PM_(2.5)的日均浓度平均值分别为76.8μg/m~3和40.0μg/m~3,均达到国家二级标准;浓度超标的天数占总观测天数的5.1%和9.3%,属污染轻微的地区。PM_(2.5)/PM_(10)在25.3%~78.8%之间周期性波动,平均值为52.1%。PM_(10)和PM_(2.5)的浓度变化具有很好的正相关性(r=0.919 8,p0.000 1);日均值在7个月中呈现明显的周期性变化,各月相对稳定,12月的PM_(10)和PM_(2.5)浓度最高且变化最为剧烈,6月最为平缓。PM_(10)和PM_(2.5)浓度小时变化总体上呈双峰型分布,最高值出现在出现在09:00—10:00和19:00—21:00前后,最低值出现在14:00—17:00之间。     

Elemental composition of PM10 and PM2.5 in urban environment in South Brazil

The purpose of the present study is to analyze the elemental composition and the concentrations of PM₁₀ and PM_2.5 in the Guaíba Hydrographic Basin with HV PM₁₀ and dichotomous samplers. Three sampling sites were selected: 8° Distrito, CEASA and Charqueadas. The sampling was conducted from October 2001 to December 2002. The mass concentrations of the samplers were evaluated, while the elemental concentrations of Si, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu and Zn were determined using the Particle-Induced X-ray Emission (PIXE) technique. Factor Analysis and Canonical Correlation Analysis were applied to the chemical and meteorological variables in order to identify the sources of particulate matter. Industrial activities such as steel plants, coal-fired power plants, hospital waste burning, vehicular emissions and soil were identified as the sources of the particulate matter. Concentration levels higher than the daily and the annual average air quality standards (150 and 50 μg m⁻³, respectively) set by the Brazilian legislation were not observed.     

Using CALINE dispersion to assess vehicular PM2.5 emissions

This paper explores the range of CALINE4's PM_2.5 modeling capabilities by comparing previously collected PM_2.5 data with CALINE4 predicted values. Two sampling sites, a suburban site located at an intersection in Sacramento, CA, and an urban site located in London, were used. Predicted concentrations are graphed against observed concentrations and evaluated against the criterion that 75% of the points fall within the factor-of-two prediction envelope. For the suburban site, data estimated by CALINE4 produced results that fell within the acceptable factor-of-two percentage envelope. A reverse dispersion test was also conducted for the suburban site using observed and calculated emission factors, and although it showed correlations between the observed values and CALINE4 predicted values, it could not conclusively prove that the model is accurate at predicting PM_2.5 concentrations. Although the results suggest that CALINE4 PM_2.5 predictions may be reasonably close to observed values, the number of observations used to verify the model was small and consequently, findings from the suburban site should be considered exploratory. For the urban site, a much larger data set was evaluated; however, the CALINE4 results for this site did not fall 75% within the factor-of-two envelope. Several factors, including street canyon effects, likely contributed to an inaccuracy of the emission factors used in CALINE4, and therefore, to the overall CALINE4 predictions. In summary, CALINE4 does not appear to perform well in densely populated areas and differences in topography may be a decisive factor in determining when CALINE4 may be applicable to modeling PM_2.5. For critical transportation projects requiring PM_2.5 analysis, use of CALINE4 may not be optimal because of its inability to produce reasonable estimates for highly trafficked areas. Additional data sets for CALINE4 analysis, particularly in urban environments, are required to fully understand CALINE4's PM_2.5 modeling capabilities.     

2015年南京市PM2.5与PM10的污染特征

分析了2015年南京市PM2.5和PM10的浓度特征和大致来源类型。PM2.5和PM10的年均浓度分别为56.6 μg·m-3和96.5 μg·m-3,污染水平较高。颗粒物浓度的季节变化特征一致：冬 > 春 > 秋 > 夏;PM2.5的日变化呈"单峰单谷"型,而PM10的呈"单峰双谷"型。颗粒物浓度在城区高于郊区;植被茂盛区域的浓度较低。对PM2.5/PM10而言,比值在冬季和梅雨期较大,分别受取暖和降水的影响;比值在春季和夏末秋初较小,分别受沙尘和秸秆焚烧的影响。PM2.5多为二次颗粒物,PM10多为一次颗粒物;固定污染源对PM2.5的间接贡献和对PM10的直接贡献较移动污染源而言更大。     

Exposure to ultrafine particles and PM2.5 in four Sydney transport modes

Concentrations of ultrafine (<0.1 μm) particles (UFPs) and PM_2.5 (<2.5 μm) were measured whilst commuting along a similar route by train, bus, ferry and automobile in Sydney, Australia. One trip on each transport mode was undertaken during both morning and evening peak hours throughout a working week, for a total of 40 trips. Analyses comprised one-way ANOVA to compare overall (i.e. all trips combined) geometric mean concentrations of both particle fractions measured across transport modes, and assessment of both the correlation between wind speed and individual trip means of UFPs and PM_2.5, and the correlation between the two particle fractions. Overall geometric mean concentrations of UFPs and PM_2.5 ranged from 2.8 (train) to 8.4 (bus) × 10⁴ particles cm^?3 and 22.6 (automobile) to 29.6 (bus) μg m^?3, respectively, and a statistically significant difference (p < 0.001) between modes was found for both particle fractions. Individual trip geometric mean concentrations were between 9.7 × 10³ (train) and 2.2 × 10⁵ (bus) particles cm^?3 and 9.5 (train) to 78.7 (train) μg m^?3. Estimated commuter exposures were variable, and the highest return trip mean PM_2.5 exposure occurred in the ferry mode, whilst the highest UFP exposure occurred during bus trips. The correlation between fractions was generally poor, and in keeping with the duality of particle mass and number emissions in vehicle-dominated urban areas. Wind speed was negatively correlated with, and a generally poor determinant of, UFP and PM_2.5 concentrations, suggesting a more significant role for other factors in determining commuter exposure.     

Effect of local and long-range transport emissions on the elemental composition of PM10–2.5 and PM2.5 in Beirut

The elemental composition of PM_10−2.5 and PM_2.5 were studied in winter, summer, stormy and non-stormy dates during a period extending from February 2004 till January 2005, in a populated area of Beirut. Results of PIXE analysis and enrichment factor (E.F.) calculation, using Si as a reference of crustal material, showed that crustal elements (E.F.<10) like Si, Ca, K, Ti, Mn and Fe were more abundant in PM_10−2.5 while enriched elements (E.F.>10) like S, Cu, Zn and Pb predominated in PM_2.5. In PM_10−2.5, concentrations of crustal elements increased during stormy episodes, all time high Ca concentrations were due to the abundance of calcite and limestone rocks in Lebanon, and increased Cl levels correlated with marine air masses. In PM_2.5, sulfur concentrations were more prominent in the summer due to the enhancement of photochemical reactions. Sources of sulfur were attributed to local, sea-water and long-range transport from Eastern Europe, with the latter being the most predominate. Anthropogenic elements like Cu and Zn were generated from worn brakes and tires in high traffic density area and spikes of Pb were directly linked to a southerly wind originated from Egypt and/or Israel as determined by the air trajectory HYSPLIT model. In brief, elemental variations depended on the regional variability of the transport pattern and the different removal rates of aerosols.