Source apportionment of wintertime secondary organic aerosol during the California regional PM10/PM2.5 air quality study

The UCD/CIT air quality model with the Caltech Atmospheric Chemistry Mechanism (CACM) was used to predict source contributions to secondary organic aerosol (SOA) formation in the San Joaquin Valley (SJV) from December 15, 2000 to January 7, 2001. The predicted 24-day average SOA concentration had a maximum value of 4.26 μg m^?3 50 km southwest of Fresno. Predicted SOA concentrations at Fresno, Angiola, and Bakersfield were 2.46 μg m^?3, 1.68 μg m^?3, and 2.28 μg m^?3, respectively, accounting for 6%, 37%, and 4% of the total predicted organic aerosol. The average SOA concentration across the entire SJV was 1.35 μg m^?3, which accounts for approximately 20% of the total predicted organic aerosol. Averaged over the entire SJV, the major SOA sources were solvent use (28% of SOA), catalyst gasoline engines (25% of SOA), wood smoke (16% of SOA), non-catalyst gasoline engines (13% of SOA), and other anthropogenic sources (11% of SOA). Diesel engines were predicted to only account for approximately 2% of the total SOA formation in the SJV because they emit a small amount of volatile organic compounds relative to other sources. In terms of SOA precursors within the SJV, long-chain alkanes were predicted to be the largest SOA contributor, followed by aromatic compounds. The current study identifies the major known contributors to the SOA burden during a winter pollution episode in the SJV, with further enhancements possible as additional formation pathways are discovered.     

South Pole Antarctica observations and modeling results: New insights on HOx radical and sulfur chemistry

Measurements of OH, H₂SO₄, and MSA at South Pole (SP) Antarctica were recorded as a part of the 2003 Antarctic Chemistry Investigation (ANTCI 2003). The time period 22 November, 2003–2 January, 2004 provided a unique opportunity to observe atmospheric chemistry at SP under both natural conditions as well as those uniquely defined by a solar eclipse event. Results under natural solar conditions generally confirmed those reported previously in the year 2000. In both years the major chemical driver leading to large scale fluctuations in OH was shifts in the concentration levels of NO. Like in 2000, however, the 2003 observational data were systematically lower than model predictions. This can be interpreted as indicating that the model mechanism is still missing a significant HO_x sink reaction(s); or, alternatively, that the OH calibration source may have problems. Still a final possibility could involve the integrity of the OH sampling scheme which involved a fixed building site. As expected, during the peak in the solar eclipse both NO and OH showed large decreases in their respective concentrations. Interestingly, the observational OH profile could only be approximated by the model mechanism upon adding an additional HO_x radical source in the form of snow emissions of CH₂O and/or H₂O₂. This would lead one to think that either CH₂O and/or H₂O₂ snow emissions represent a significant HO_x radical source under summertime conditions at SP. Observations of H₂SO₄ and MSA revealed both species to be present at very low concentrations (e.g., 5 × 10⁵ and 1 × 10⁵ molec cm^?3, respectively), but similar to those reported in 2000. The first measurements of SO₂ at SP demonstrated a close coupling with the oxidation product H₂SO₄. The observed low concentrations of MSA appear to be counter to the most recent thinking by glacio-chemists who have suggested that the plateau's lower atmosphere should have elevated levels of MSA. We speculate here that the absence of MSA may reflect efficient atmospheric removal mechanisms for this species involving either dynamical and/or chemical processes.     

Characteristics of springtime profiles and sources of ozone in the low troposphere over northern Taiwan

To quantify the possible sources of the high ambient ozone concentration in the low troposphere over Taiwan, ozone sounding data from a two-year intensive field measurement program conducted in April and early May of 2004 and 2005 in northern Taiwan has been examined. We found that the vertical ozone distributions and occurrence of enhanced ozone in the lower troposphere (below 6 km) mainly resulted from (1)Type NE: the long-range transport of ozone controlled by the prevailing northeasterly winds below 2 km, (2)Type LO: the local photochemical ozone production process, and (3)Type SW: the strong southwest/westerly winds aloft (2–6 km). In the boundary layer (BL), where Asian continental outflow prevails, the average profile for type NE is characterized by a peak ozone concentration of nearly 65 ppb at about 1500 m altitude. For type LO, high ozone concentration with an average ozone concentration greater than 80 ppb was also found in the BL in the case of stagnant atmospheric and sunny weather conditions dominated. For type SW, significant ozone enhancement with average ozone concentration of 70–85 ppb was found at around 4 km altitude. It is about 10 ppb greater than that of the types NE and LO at the same troposphere layer owing to the contribution of the biomass burning over Indochina. Due to Taiwan's unique geographic location, the complex interaction of these ozone features in the BL and aloft, especially features associated with northeasterly and south/southwesterly winds, have resulted in complex characteristics of ozone distributions in the lower troposphere over northern Taiwan.     

两阶段曝气生物滤池的硝化性能

曝气生物滤池(BAF)是近年来受到广泛关注的一种新型污水处理技术,具有占地面积少、投资费用低、处理效率高、出水水质好等优点。现已被应用于许多污水处理厂的二级处理、深度处理以及污水的回用。实验以陶粒为填料,自行设计了升流式两阶段BAFs(UBAFs)处理模拟生活污水,考察了反应器运行条件对COD与氨氮去除影响,并探讨了UBAFs反应器内氮流失及同步硝化反硝化情况。结果表明,UBAFs对生活污水处理具有良好的净化效果。在进水COD和氨氮浓度分别为200~363 mg/L和16.8~31.3 mg/L条件下,UBAFs处理出水水质均达到《城市污水再生利用城市杂用水水质》(GB/T 18920-2002)标准,能够满足回用要求。通过采用氮平衡分析方法和借助电子扫描电镜技术,初步认为UBAFs反应器脱氮方式是由于在UBAFs第一阶段局部厌氧环境中以传统方式进行硝化反硝化脱氮,第二阶段是在好氧条件下,异养好氧硝化菌的同步硝化反硝化脱氮。     

ACF电极电解处理含NaCl结晶紫染料废水的研究

以吸附结晶紫达到饱和的活性炭纤维为阳极,在NaCl介质中对初始浓度为100 mg/L的结晶紫染料废水进行了电解脱色处理。实验考察了NaCl浓度、pH值和电流密度等对溶液脱色率的影响,测定了电解时溶液中生成的游离氯浓度及不同电解时间后溶液的紫外-可见吸收光谱曲线,并对不同电解时间后溶液的归一化吸光度比值进行了计算。结果发现,溶液中所产生的游离氯的浓度随电解时间的增加快速上升,20 min时就几乎达到了最大值;在活性氯的作用下,结晶紫分子中的大π共轭体系被破坏,溶液迅速脱色;电解液中所含的NaCl浓度、电解液的pH值和电流密度等都对脱色率有影响;在一定实验条件下,初始浓度为100 mg/L的结晶紫染料废水在电解60 min后脱色率可高达99.3%。     

Atmospheric deposition of phthalate esters in a subtropical city

In Chinese cities, air pollution has become a serious and aggravating environmental problem undermining the sustainability of urban ecosystems and the quality of urban life. Bulk atmospheric deposition samples were collected two-weekly, from February 2007 to January 2008, at three representative areas, one suburban and two urbanized, in the subtropical city, Guangzhou, China, to assess the deposition fluxes and seasonal variations of phthalate esters (PAEs). Sixteen PAE congeners in bulk deposition samples were measured and the depositional fluxes of ∑₁₆PAEs ranged from 3.41 to 190 μg m^?2 day^?1, and were highly affected by local anthropogenic activities. The significant relationship between PAEs and particulate depositional fluxes (correlation coefficient R² = 0.72, P < 0.001) showed PAEs are associated primarily with particles. Temporal flux variations of PAEs were influenced by seasonal changes in meteorological parameters, and the deposition fluxes of PAEs were obviously higher in wet season than in dry season. Diisobutyl phthalate (DiBP), Di-n-butyl phthalate (DnBP), and Di(2-ethylhexyl) phthalate (DEHP) dominated the PAE pattern in bulk depositions, which is consistent with a high consumption of the plasticizer market in China. PAE profiles in bulk deposition showed similarities exhibited in both time and space, and a weak increase of high molecular weight PAE (HMW PAE) contribution in the wet season compared to those in the dry season. Average atmospheric deposition fluxes of PAEs in the present study were significantly higher than those from other studies, reflecting strong anthropogenic inputs as a consequence of rapid industrial and urban development in the region.     

Estimation of economic costs of particulate air pollution from road transport in China

Valuation of health effects of air pollution is becoming a critical component of the performance of cost–benefit analysis of pollution control measures, which provides a basis for setting priorities for action. Beijing has focused on control of transport emission as vehicular emissions have recently become an important source of air pollution, particularly during Olympic games and Post-games. In this paper, we conducted an estimation of health effects and economic cost caused by road transport-related air pollution using an integrated assessment approach which utilizes air quality model, engineering, epidemiology, and economics. The results show that the total economic cost of health impacts due to air pollution contributed from transport in Beijing during 2004–2008 was 272, 297, 310, 323, 298 million US$ (mean value), respectively. The economic costs of road transport accounted for 0.52, 0.57, 0.60, 0.62, and 0.58% of annual Beijing GDP from 2004 to 2008. Average cost per vehicle and per ton of PM₁₀ emission from road transport can also be estimated as 106 US $/number and 3584 US $ t^?1, respectively. These findings illustrate that the impact of road transport contributed particulate air pollution on human health could be substantial in Beijing, whether in physical and economic terms. Therefore, some control measures to reduce transport emissions could lead to considerable economic benefit.     

Simple model for estimating dry deposition velocity of ozone and its destruction in a polluted nocturnal boundary layer

Determining the destructions of both ozone and odd oxygen, O_x, in the nocturnal boundary layer (NBL) is important to evaluate the regional ozone budget and overnight ozone accumulation. This work develops a simple method to determine the dry deposition velocity of ozone and its destruction at a polluted nocturnal boundary layer. The destruction of O_x can also be determined simultaneously. The method is based on O₃ and NO₂ profiles and their surface measurements. Linkages between the dry deposition velocities of O₃ and NO₂ and between the dry deposition loss of O_x and its chemical loss are constructed and used. Field measurements are made at an agricultural site to demonstrate the application of the model. The model estimated nocturnal O₃ dry deposition velocities from 0.13 to 0.19 cm s^?1, very close to those previously obtained for similar land types. Additionally, dry deposition and chemical reactions account for 60 and 40% of the overall nocturnal ozone loss, respectively; ozone dry deposition accounts for 50% of the overall nocturnal loss of O_x, dry deposition of NO₂ accounts for another 20%, and chemical reactions account for the remaining 30%. The proposed method enables the use of measurements made in typical ozone field studies to evaluate various nocturnal destructions of O₃ and O_x in a polluted environment.     

Chemical mass balance source apportionment for combined PM2.5 measurements from U.S. non-urban and urban long-term networks

The Minnesota Particulate Matter 2.5 (PM_2.5) Source Apportionment Study was undertaken to explore the utility of PM_2.5 mass, element, ion, and carbon measurements from long-term speciation networks for pollution source attribution. Ambient monitoring data at eight sites across the state were retrieved from the archives of the Interagency Monitoring of Protected Visual Environments (IMPROVE) and the Speciation Trends Network (STN; part of the Chemical Speciation Network [CSN]) and analyzed by an Effective Variance – Chemical Mass Balance (EV-CMB) receptor model with region-specific geological source profiles developed in this study. PM_2.5 was apportioned into contributions of fugitive soil dust, calcium-rich dust, taconite (low grade iron ore) dust, road salt, motor vehicle exhaust, biomass burning, coal-fired utility, and secondary aerosol. Secondary sulfate and nitrate contributed strongly (49–71% of PM_2.5) across all sites and was dominant (≥60%) at IMPROVE sites. Vehicle exhausts accounted for 20–70% of the primary PM_2.5 contribution, largely exceeding the proportion in the primary PM_2.5 emission inventory. The diesel exhaust contribution was separable from the gasoline engine exhaust contribution at the STN sites. Higher detection limits for several marker elements in the STN resulted in non-detectable coal-fired boiler contributions which were detected in the IMPROVE data. Despite the different measured variables, analytical methods, and detection limits, EV-CMB results from a nearby IMPROVE-STN non-urban/urban sites showed similar contributions from regional sources – including fugitive dust and secondary aerosol. Seasonal variations of source contributions were examined and extreme PM_2.5 episodes were explained by both local and regional pollution events.     

Emission factors and particulate matter size distribution of polycyclic aromatic hydrocarbons from residential coal combustions in rural Northern China

Coal consumption is one important contributor to energy production, and is regarded as one of the most important sources of air pollutants that have considerable impacts on human health and climate change. Emissions of polycyclic aromatic hydrocarbons (PAHs) from coal combustion were studied in a typical stove. Emission factors (EFs) of 16 EPA priority PAHs from tested coals ranged from 6.25 ± 1.16 mg kg^?1 (anthracite) to 253 ± 170 mg kg^?1 (bituminous), with NAP and PHE dominated in gaseous and particulate phases, respectively. Size distributions of particulate phase PAHs from tested coals showed that they were mostly associated with particulate matter (PM) with size either between 0.7 and 2.1 μm or less than 0.4 μm (PM_0.4). In the latter category, not only were more PAHs present in PM_0.4, but also contained higher fractions of high molecular weight PAHs. Generally, there were more than 89% of total particulate phase PAHs associated with PM_2.5. Gas-particle partitioning of freshly emitted PAHs from residential coal combustions were thought to be mainly controlled by absorption rather than adsorption, which is similar to those from other sources. Besides, the influence of fuel properties and combustion conditions was further investigated by using stepwise regression analysis, which indicated that almost 57 ± 10% of total variations in PAH EFs can be accounted for by moisture and volatile matter content of coal in residential combustion.