Determination of Source Contributions to Ambient PM2.5 in Kaohsiung,Taiwan, Using a Receptor Model

ABSTRACT

Ambient particulates of PM_2.5 were sampled at three sites in Kaohsiung, Taiwan, during February and March 1999. In addition, resuspended PM_2.5 collected from traffic tunnels, paved roads, fly ash of a municipal solid waste (MSW) incinerator, and seawater was obtained. All the samples were analyzed for twenty constituents, including water-soluble ions, organic carbon (OC), elemental carbon (EC), and metallic elements. In conjunction with local source profiles and the source profiles in the model library SPECIATE EPA, the receptor model based on chemical mass balance (CMB) was then applied to determine the source contributions to ambient PM_2.5.

The mean concentration of ambient PM_2.5 was 42.6953.68 μj.g/m³ for the sampling period. The abundant species in ambient PM_2.5 in the mass fraction for three sites were OC (12.7-14.2%), SO₄ ^2- (12.8-15.1%), NO₃ ^- (8.110.3%), NH₄+ (6.7-7.5%), and EC (5.3-8.5%). Results of CMB modeling show that major pollution sources for ambient PM_2.5 are traffic exhaust (18-54%), secondary aerosols (30-41% from SO₄ ^2- and NO₃ ^-), and outdoor burning of agriculture wastes (13-17%).     

Determination of source contributions to ambient PM2.5 in Kaohsiung, Taiwan, using a receptor model

Ambient particulates of PM2.5 were sampled at three sites in Kaohsiung, Taiwan, during February and March 1999. In addition, resuspended PM2.5 collected from traffic tunnels, paved roads, fly ash of a municipal solid waste (MSW) incinerator, and seawater was obtained. All the samples were analyzed for twenty constituents, including water-soluble ions, organic carbon (OC), elemental carbon (EC), and metallic elements. In conjunction with local source profiles and the source profiles in the model library SPECIATE EPA, the receptor model based on chemical mass balance (CMB) was then applied to determine the source contributions to ambient PM2.5. The mean concentration of ambient PM2.5 was 42.69-53.68 micrograms/m3 for the sampling period. The abundant species in ambient PM2.5 in the mass fraction for three sites were OC (12.7-14.2%), SO4(2-) (12.8-15.1%), NO3- (8.1-10.3%), NH4+ (6.7-7.5%), and EC (5.3-8.5%). Results of CMB modeling show that major pollution sources for ambient PM2.5 are traffic exhaust (18-54%), secondary aerosols (30-41% from SO4(2-) and NO3-), and outdoor burning of agriculture wastes (13-17%).     

Effects of aerosol species on atmospheric visibility in Kaohsiung City, Taiwan

Visibility data collected from Kaohsiung City, Taiwan, for the past two decades indicated that the air pollutants have significantly degraded visibility in recent years. During our study period, the seasonal mean visibilities in spring, summer, fall, and winter were only 5.4, 9.1, 8.2, and 3.4 km, respectively. To ascertain how urban aerosols influence the visibility, we conducted concurrent visibility monitoring and aerosol sampling in 1999 to identify the principal causes of visibility impairments in the region. In this study, ambient aerosols were sampled and analyzed for 11 constituents, including water-soluble ions and carbon materials, to investigate the chemical composition of Kaohsiung aerosols. Stepwise regression method was used to correlate the impact of aerosol species on visibility impairments. Both seasonal and diurnal variation patterns were found from the monitoring of visibility. Our results showed that light scattering was attributed primarily to aerosols with sizes that range from 0.26 to 0.90 pm, corresponding with the wavelength region of visible light, which accounted for approximately 72% of the light scattering coefficient. Sulfate was a dominant component that affected both the light scattering coefficient and the visibility in the region. On average, (NH4)2SO4, NH4NO3, total carbon, and fine particulate matter (PM2.5)-remainder contributed 53%, 17%, 16%, and 14% to total light scattering, respectively. An empirical regression model of visibility based on sulfate, elemental carbon, and humidity was developed, and the comparison indicated that visibility in an urban area could be properly simulated by the equation derived herein.     

Concentrations and distributions of carbonaceous species in ambient particles in Kaohsiung City,Taiwan

Concentrations and distributions of elemental carbon (EC) and organic carbon (OC) in particles were measured in Kaohsiung City, Taiwan. PM₁₀ and PM_2.5 samples were collected using a dichotomous sampler from November 1998 to April 1999 and were analyzed for carbonaceous species with an elemental analyzer. The concentrations of carbonaceous species in Kaohsiung City were comparable to those at other urban locations in the world. On average, carbonaceous species accounted for 21.2% of the PM_2.5 and 18.1% of the PM₁₀. It was found that organic carbon dominated the carbonaceous species and was 72.2 and 70.4% of total carbon (TC) for PM_2.5 and PM₁₀. The secondary organic carbon formed through the volatile organic compound gas-to-particle conversion was estimated from the minimum ratio between elemental and organic carbon obtained in this study, and was found to constitute 40.0 and 32.4% of the total organic carbon particle for PM_2.5 and PM₁₀ (or 6.6 and 4.5% of the total particle mass).     

Characterization of carbonaceous species of ambient PM2.5 in Beijing, China

One-week integrated fine particulate matter (i.e., particles <2.5 microm in diameter; PM2.5) 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 microg 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 approximately 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.     

Characterization of atmospheric PM10 and related chemical species in southern Taiwan during the episode days

The concentrations of atmospheric PM10 on days with episodes of pollution were examined at four different sampling sites (CC, DL, LY, and HK) in southern Taiwan. The related to particulates water-soluble ionic species (Na+, K+, Mg2+, Ca2+, NH4+, Cl-, NO3-, SO4(2-)), carbonaceous species (EC and OC) and metallic species (Zn, Ni, Pb, Fe, Mn, Al, Si, V) were also analyzed. On the episode days of this study, the PM10 mass concentration ranged from 155 to 210 microgm(-3), from 150 to 208 microgm(-3), from 182 to 249 microgm(-3), and from 166 to 228 microgm(-3) at CC, DL, LY, and HK, respectively. The results indicate that the dominant water-soluble species were SO4(2-), NO3-, NH4+, and Cl- at the four sampling sites on these days. Moreover, the high sulfate and nitrate conversion values (SOR and NOR) presented herein suggest that secondary formations from SO2 to SO4(2-) and from NO2 to NO3- are present in significant quantities in the atmosphere of southern Taiwan on episode days. In particular, high SOR and NOR verified that both SO4(2-) and NO3- dominated the increase of atmospheric PM10 concentration in southern Taiwan on episode days.     

Characterization of carbonaceous species in PM2.5 in Xi'an during spring

The characterization of carbonaceous species in PM_2.5 during a spring period in a suburb of Xi'an, China was investigated. PM_2.5 samples were collected on quartz filters and analyzed for organic carbon (OC) and elemental carbon (EC). The thermal optical reflectance method was used. The minimum OC/EC ratio method was used to estimate the concentration of secondary organic carbon (SOC). The distribution of eight carbon fractions was investigated as well. The average mass concentrations of OC and EC were 15.90 and 8.38 μg/m³, respectively. The average OC/EC ratio ranged from 1.16 to 3.16 with an average value of 2.25. This implies the existence of SOC in PM_2.5. The mean SOC concentration was 7.20 μg/m³, accounting for 45.28% of total OC. This result suggests that SOC is a significant component of OC in the suburb of Xi'an. Results from the distribution of eight carbon fractions revealed that emissions from motor vehicle, coal combustion, and road dust were the main source of carbonaceous particles in the sampling period.     

High occurrence of BTEX around major industrial plants in Kaohsiung,Taiwan

The Houjing River, which flows by large industrial complexes in southwestern Taiwan, has been seriously polluted with benzene, toluene, ethylbenzene, and xylene (BTEX). Using Spearman’s analysis of BTEX concentrations measured at different sites along the river, we identified the main sources of this pollution to be the Dashe and Renwu Industrial Parks. Maximum concentrations of benzene and toluene (402 and 143.19 µg/L, respectively) were considerably higher than those reported in similar studies and regulatory limits. We compared these findings with those of positive matrix factorization (PMF) modelling. PMF also identified the two industrial parks as being sources of BTEX, most likely originating from petrochemical activities that occur there. This study can serve as an important reference for future watershed management and pollution control plans for Kaohsiung, the most industrialized city in Taiwan. PMF proved to be a reliable computer modelling program for source apportionment and environmental forensic studies.     

Effects of Aerosol Species on Atmospheric Visibility in Kaohsiung City,Taiwan

Abstract

Visibility data collected from Kaohsiung City, Taiwan, for the past two decades indicated that the air pollutants have significantly degraded visibility in recent years. During our study period, the seasonal mean visibilities in spring, summer, fall, and winter were only 5.4, 9.1, 8.2, and 3.4 km, respectively. To ascertain how urban aerosols influence the visibility, we conducted concurrent visibility monitoring and aerosol sampling in 1999 to identify the principal causes of visibility impairments in the region. In this study, ambient aerosols were sampled and analyzed for 11 constituents, including water-soluble ions and carbon materials, to investigate the chemical composition of Kaohsiung aerosols. Stepwise regression method was used to correlate the impact of aerosol species on visibility impairments. Both seasonal and diurnal variation patterns were found from the monitoring of visibility. Our results showed that light scattering was attributed primarily to aerosols with sizes that range from 0.26 to 0.90 μm, corresponding with the wavelength region of visible light, which accounted for ～72% of the light scattering coefficient. Sulfate was a dominant component that affected both the light scattering coefficient and the visibility in the region. On average, (NH₄)₂SO₄, NH₄NO₃, total carbon, and fine particulate matter (PM_2.5)-remainder contributed 53%, 17%, 16%, and 14% to total light scattering, respectively. An empirical regression model of visibility based on sulfate, elemental carbon, and humidity was developed, and the comparison indicated that visibility in an urban area could be properly simulated by the equation derived herein.     

The study of TSP, PM(2.5-10) and PM2.5 during Taiwan Chi-Chi Earthquake in the traffic site of central Taiwan, Taichung

Ambient particle concentration was taken on the traffic sampling site over the Chung-Chi Road over bridge (CCROB) in front of Hungkuang Institute of Technology (HKIT). The sampling time was from August 1999 to December 1999. During the sampling period, Taiwan's biggest earthquake in more than a century registered 7.3 on the Richter scale (Taiwan Chi-Chi Earthquake). Besides, there were more than 20,000 aftershocks that followed the Taiwan Chi-Chi Earthquake within three months. Thus, the PM2.5, PM(2.5-10) particle concentrations were also collected then and compared with total suspended particle (TSP) in this study. The average PM(2.5-10), PM2.5 and TSP concentrations are 24.6, 58.0 and 106 microg/m3, respectively, after the Taiwan Chi-Chi Earthquake. The average TSP concentrations before and after Taiwan Chi-Chi Earthquake were 70 and 127 microg/m3, respectively. It is clearly shown that the average concentration of TSP after Taiwan Chi-Chi Earthquake was about 1.8 times as that of TSP concentration before Taiwan Chi-Chi Earthquake in the traffic site of central Taiwan. And the ratios of PM2.5/PM(2.5-10), PM2.5/PM10 and PM2.5/TSP are 2.2%, 67.2%, 38.9%, respectively. The results also indicated about Chi-Chi fine particle concentration (PM25) and the TSP increases in the traffic site of central Taiwan after Taiwan Chi-Chi Earthquake.     

Characteristics of the major chemical constituents of PM2.5 and smog events in Seoul,Korea in 2003 and 2004

One hundred ninety-five chemically speciated samples were collected from March 2003 to February 2005 in the Seoul Metropolitan area to investigate the characteristics of the major components in PM_2.5 and to characterize the chemical variations between smog and non-smog events. The annual average PM_2.5 concentration was 43 μg m⁻³ that is almost three times higher than the US NAAQS annual PM_2.5 standard of 15 μg m⁻³. During this sampling period, smog and yellow sand events were observed on 27 and 10 days, respectively. The PM_2.5 concentrations and its constituents during smog events were about two–three times higher than those during non-smog and yellow sand events. In particular, the mass fractions of secondary aerosols such as sulfate, nitrate, and ammonium during the smog events were higher than those of the other constituents. The mean concentration and mass fraction of secondary organic carbon (SOC) were highest during the winter smog events. Sulfate, nitrate and SOC that can have long residence times were important species during the smog events suggesting that regional scale sources rather than local sources were important. Five-day backward air trajectory analysis showed that the air parcels during smog events passed through the major industrial areas in China more often than those during non-smog events.     

Characterization of n-alkanes in PM2.5 of the Taipei aerosol

Ambient concentrations of n-alkanes with carbon number ranging from 17 to 36 were determined for PM_2.5 samples collected in Taipei city during September 1997–February 1998. The measured concentrations of particulate n-alkanes were in the range of 69–702 ng m⁻³, considerably higher than the concentration levels observed in Los Angeles and Hong Kong. The concentration distributions of n-alkanes homologues obtained in this study exhibited peaks at C₁₉, C₂₄ or C₂₅. This suggests that fossil fuel utilization, such as vehicular exhaust and lubricant residues, was an important contributor to the Taipei aerosol. Source apportionment of PM_2.5 was conducted using carbon preference index (CPI, defined as the ratio of the total concentration of particulate n-alkanes with odd carbon number to that with even carbon number) and U : R ratio (the concentration ratio of unresolved components to resolved components obtained from chromatograms). The low CPI value (0.9–1.9) and high U : R ratio (2.6–6.4) for each sample further confirmed that fossil fuel utilization was the major source of n-alkanes in ambient PM_2.5 of Taipei city. Estimates from these results showed that 69–93% of the n-alkanes in PM_2.5 of the Taipei aerosol originated from vehicular exhaust. The higher concentration level of particulate n-alkanes in the Taipei aerosol was mainly a result of vehicular emissions.     

Chemical characteristics of principal PM2.5 species in Chongju,South Korea

Fine particles were collected over four seasons from October 1995 to August 1996 to evaluate the chemical characteristics of principal PM_2.5 components in Chongju, South Korea. The annual mean concentrations of PM_2.5 (d_p⩽2.5 μm), sulfate, nitrate, ammonium, elemental carbon (EC) and organic carbon (OC) were 44.2, 8.22, 3.63, 2.84, 4.44 and 4.99 μg m⁻³, respectively. The sum of the species measured from this study accounted for 50–62% of the PM_2.5 mass. Sulfate was the most abundant species and constituted 13–23% of the PM_2.5 mass. The EC and OC accounted for 17–28% of PM_2.5. The correlation between OC and EC was strong, and the annual mean ratio of OC/EC was 1.12, suggesting that OC measured in the Chongju area may be emitted directly in particulate form as a primary aerosol.     

忻州市大气PM2.5的化学组成质量平衡特征及来源解析

于2013年9月（非采暖季）、2014年2-3月（采暖季）、2014年5月（风沙季）采集忻州市3个监测点（新城区、开发区和旧城区）的PM2.5样品,分析其中的39种元素、9种水溶性离子及2种碳组分,并对PM2.5的质量浓度进行重构。结果表明,重构后的化学组分分为5类：矿物尘、微量元素、有机物、元素碳和二次粒子,其中矿物尘、二次粒子及有机物是忻州PM2.5的主要组成,分别占到ρ（PM2.5）的24.0%~36.2%、19.2%~32.6%和12.9%~25.7%;化学组成质量分数具有较明显的季节变化特征,风沙季矿物尘质量分数高于采暖季和非采暖季,采暖季有机物质量分数高于其他两季,非采暖季二次粒子质量分数略高于其他两季;化学组分的空间变化显示会展中心站点的二次粒子和矿物尘质量分数明显高于其他2个站点。应用化学质量平衡（CMB）模型进行来源解析,结果显示忻州市PM2.5的主要来源是扬尘（21%~35%）、二次粒子（25%~26%）和机动车尾气（21%~26%）。     

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.     

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.     

Characteristics of vertical profiles and sources of PM2.5, PM10 and carbonaceous species in Beijing

In August 2003 during the anticipated month of the 2008 Beijing Summer Olympic Games, we simultaneously collected PM₁₀ and PM_2.5 samples at 8, 100, 200 and 325 m heights up a meteorological tower and in an urban and a suburban site in Beijing. The samples were analysed for organic carbon (OC) and elemental carbon (EC) contents. Particulate matter (PM) and carbonaceous species pollution in the Beijing region were serious and widespread with 86% of PM_2.5 samples exceeding the daily National Ambient Air Quality Standard of the USA (65 μg m⁻³) and the overall daily average PM₁₀ concentrations of the three surface sites exceeding the Class II National Air Quality Standard of China (150 μg m⁻³). The maximum daily PM_2.5 and PM₁₀ concentrations reached 178.7 and 368.1 μg m⁻³, respectively, while those of OC and EC reached 22.2 and 9.1 μg m⁻³ in PM_2.5 and 30.0 and 13.0 μg m⁻³ in PM₁₀, respectively. PM, especially PM_2.5, OC and EC showed complex vertical distributions and distinct layered structures up the meteorological tower with elevated levels extending to the 100, 200 and 300 m heights. Meteorological evidence suggested that there exist fine atmospheric layers over urban Beijing. These layers were featured by strong temperature inversions close to the surface (<50 m) and more stable conditions aloft. They enhanced the accumulation of pollutants and probably caused the complex vertical distributions of PM and carbonaceous species over urban Beijing. The built-up of PM was accompanied by transport of industrial emissions from the southwest direction of the city. Emissions from road traffic and construction activities as well as secondary organic carbon (SOC) are important sources of PM. High OC/EC ratios (range of 1.8–5.1 for PM_2.5 and 2.0–4.3 for PM₁₀) were found, especially in the higher levels of the meteorological tower suggesting there were substantial productions of SOC in summer Beijing. SOC is estimated to account for at least 33.8% and 28.1% of OC in PM_2.5 and PM₁₀, respectively, with higher percentages at the higher levels of the tower.     

南宁市大气颗粒物TSP、PM10、PM2.5污染水平研究

2002年在南宁市的5个典型城市功能区内,共采集了125个大气样品(按季节分别采集),初步调查了大气中颗粒物TSP、PM10、PM2.5的污染状况。结果表明,南宁市TSP、PM10、PM2.5的污染很严重,超标率分别为67．5％、82．5％、92．5％,对人体健康危害更大的PM2．5占到了PM10的63．5％左右。重污染区PM2.5的浓度超过轻污染区近一倍。     

北京市2014年PM2.5质量浓度变化特征

利用北京市发布的PM2.5质量浓度数据,分析了2014年PM2.5日平均质量浓度变化情况,以及全年平均日变化特征、分季节的日变化特征、分星期的日变化特征。结果表明：北京市2014年PM2.5污染较为严重,但相比往年有所减弱,其中2月和10月污染最为严重,5-6月及8-9月污染较轻。全年平均日变化呈现“W”型,白天在07：00和15：00存在2个谷值,峰值出现在10：00,21：00-03：00 PM2.5污染在一天中最为严重。秋冬季节的日变化趋势相似,其夜间PM2.5质量浓度明显高于白天。春季和夏季的日变化与全年平均日变化差别很大。分星期的日变化曲线变化趋势存在较大差异,但峰值和谷值出现的时间基本一致。