Retained nitrate, hydrated sulfates, and carbonaceous mass in federal reference method fine particulate matter for six eastern U.S. cities

Material balance of fine particulate matter (PM2.5) measured with the Federal Reference Method (FRM) is developed for one rural and five urban locations in the eastern half of the United States using routine Speciation Trends Network (STN) and FRM chemical measurements and thermodynamic models. The Aerosol Inorganics Model is used to estimate retained particle bound water, and an ammonium nitrate evaporation model is used to estimate nitrate concentrations retained on the Teflon-membrane filter of the FRM. To address large uncertainties in carbonaceous mass calculated from STN carbon measurements, retained carbonaceous mass is derived by material balance between PM2.5 FRM mass and estimates of its non-carbon constituents. The resulting sulfate, adjusted nitrate, derived water, inferred carbonaceous material balance approach (SANDWICH) is compared with reconstructed fine mass (RCFM) using the Interagency Monitoring of Protected Visual Environments monitoring program equation. For this study, the SANDWICH method resulted in approximately 21-27% higher sulfate mass and approximately 24-85% lower nitrate mass. The combined mass associated with sulfates and nitrates, however, are well within +/- 10% of the proportion derived using the more traditional RCFM method. The discrepancies between SANDWICH and measurement-derived carbonaceous mass vary from -21% to +56% on an annual basis and are attributed in part to urban-rural source influences and uncertainties in estimating FRM-retained carbonaceous mass.     

Performance and diagnostic evaluation of ozone predictions by the Eta-Community Multiscale Air Quality Forecast System during the 2002 New England Air Quality Study

A real-time air quality forecasting system (Eta-Community Multiscale Air Quality [CMAQ] model suite) has been developed by linking the National Centers for Environmental Estimation Eta model to the U.S. Environmental Protection Agency (EPA) CMAQ model. This work presents results from the application of the Eta-CMAQ modeling system for forecasting ozone (O3) over the Northeastern United States during the 2002 New England Air Quality Study (NEAQS). Spatial and temporal performance of the Eta-CMAQ model for O3 was evaluated by comparison with observations from the EPA Air Quality System (AQS) network. This study also examines the ability of the model to simulate the processes governing the distributions of tropospheric O3 on the basis of the intensive datasets obtained at the four Atmospheric Investigation, Regional Modeling, Analysis, and Estimation (AIRMAP) and Harvard Forest (HF) surface sites. The episode analysis reveals that the model captured the buildup of O3 concentrations over the northeastern domain from August 11 and reproduced the spatial distributions of observed O3 very well for the daytime (8:00 p.m.) of both August 8 and 12 with most of normalized mean bias (NMB) within +/- 20%. The model reproduced 53.3% of the observed hourly O3 within a factor of 1.5 with NMB of 29.7% and normalized mean error of 46.9% at the 342 AQS sites. The comparison of modeled and observed lidar O3 vertical profiles shows that whereas the model reproduced the observed vertical structure, it tended to overestimate at higher altitude. The model reproduced 64-77% of observed NO2 photolysis rate values within a factor of 1.5 at the AIRMAP sites. At the HF site, comparison of modeled and observed O3/nitrogen oxide (NOx) ratios suggests that the site is mainly under strongly NOx-sensitive conditions (>53%). It was found that the modeled lower limits of the O3 production efficiency values (inferred from O3-CO correlation) are close to the observations.     

Resolving neighborhood scale in air toxics modeling: a case study in Wilmington, CA

Air quality modeling is useful for characterizing exposures to air pollutants. Whereas models typically provide results on regional scales, new concerns regarding the potential for differential exposures among racial/ethnic populations and income strata within communities are driving the need for increasingly refined modeling approaches. These approaches need to be capable of resolving concentrations on the scale of tens of meters, across modeling domains 10-100 km2 in size. One approach for refined air quality modeling is to combine Gaussian and regional photochemical grid models. In this paper, the authors demonstrate this approach on a case study of Wilmington, CA, focused on diesel exhaust particulate matter. Modeling results suggest that pollutant concentrations in the vicinity of emission sources are elevated, and, therefore, an understanding of local emission sources is necessary to generate credible modeling results. A probabilistic evaluation of the Gaussian model application indicated that spatial allocation, emission rates, and meteorological data are important contributors to input and parameter uncertainty in the model results. This uncertainty can be substantially reduced through the collection and integration of site-specific information about the location of emission sources and the activity and emission rates of key sources affecting model concentrations.     

Refining fire emissions for air quality modeling with remotely sensed fire counts: A wildfire case study

This paper examines the use of Moderate Resolution Imaging Spectroradiometer (MODIS) observed active fire data (pixel counts) to refine the National Emissions Inventory (NEI) fire emission estimates for major wildfire events. This study was motivated by the extremely limited information available for many years of the United States Environmental Protection Agency (US EPA) NEI about the specific location and timing of major fire events. The MODIS fire data provide twice-daily snapshots of the locations and breadth of fires, which can be helpful for identifying major wildfires that typically persist for a minimum of several days. A major wildfire in Mallory Swamp, FL, is used here as a case study to test a reallocation approach for temporally and spatially distributing the state-level fire emissions based on the MODIS fire data. Community Multiscale Air Quality (CMAQ) model simulations using these reallocated emissions are then compared with another simulation based on the original NEI fire emissions. We compare total carbon (TC) predictions from these CMAQ simulations against observations from the Inter-agency Monitoring of Protected Visual Environments (IMPROVE) surface network. Comparisons at three IMPROVE sites demonstrate substantial improvements in the temporal variability and overall correlation for TC predictions when the MODIS fire data is used to refine the fire emission estimates. These results suggest that if limited information is available about the spatial and temporal extent of a major wildfire fire, remotely sensed fire data can be a useful surrogate for developing the fire emissions estimates for air quality modeling purposes.     

Unsaturated dicarbonyl products from the OH-initiated photo-oxidation of furan, 2-methylfuran and 3-methylfuran

This study presents the application of O-(2,3,4,5,6)-pentafluorobenzyl-hydroxylamine hydrochloride (PFBHA) on-fibre derivatisation Solid Phase Microextraction (SPME) to the sampling and quantification of the unsaturated 1,4-dicarbonyl products obtained in the photo-oxidation of furan, 2-methylfuran and 3-methylfuran with HONO: butenedial, 4-oxo-2-pentenal and 2-methylbutenedial, respectively. The use of Proton Transfer Reaction Mass Spectrometry (PTR-MS) is also considered and the advantages of the combined use of both methodologies is discussed. The 1,4 unsaturated dicarbonyl products sampled by SPME were quantified by GC-FID.The experiments were carried out in the EUPHORE outdoor simulation chambers. The results confirm that 1,4-dicarbonyls are the main products of the OH-initiated oxidation of furan and its methylated derivatives, a fact with environmental implications. Molar yields of (1.09 ± 0.41) and (0.90 ± 0.36) were obtained in two experiments of furan photo-oxidation. The yields of 4-oxo-2-pentenal and methylbutenedial were estimated to be (0.60 ± 0.24) and (0.83 ± 0.33) respectively, assuming the same SPME response factor as for butenedial. Furthermore, the unsaturated 1,4-dicarbonyls have also been identified in the chemical characterisation of the aerosols formed in the reactions. The yield of aerosols quantified were (8.5 ± 0.8)% in the photo-oxidation of furan, (1.85 ± 0.18)% in the photo-oxidation of 2-methylfuran and (5.5 ± 0.5)% in the photo-oxidation of 3-methylfuran, at the following concentrations of their precursors: 829 ± 249 ppbV and 748 ± 224 (in two furan experiments), 633 ± 190 in the 2-methylfuran and 641 ± 192 ppbV in the 3-methylfuran experiment.     

典型城市臭氧污染源贡献及控制策略费效评估

东莞是珠三角O_3污染最严重的城市,使用RSM/CMAQ(曲面响应模型)法分析了珠三角区域人为排放的NO_x和VOCs对东莞市O_3浓度变化源贡献.2014基准年分析结果表明,扣除模型域外区域传输及天然源排放对O_3本底浓度贡献(41.00%)后,东莞本地VOCs排放对O_3贡献最大(18.50%),珠三角区域NO_x减排率13%时可持续降低东莞市O_3浓度.进一步使用ABa CAS-SE(空气污染控制成本效益与达标评估系统)对2017、2020、2025东莞市3个未来年O_3污染控制情景进行了费效评估.评估结果显示,NO_x和VOCs控制比例相对较低的2017年控制情景人体健康效益/区域控制成本比约为1.1;而控制比例相对较高的2025年东莞O_3达标情景效益成本比仅为0.1.这说明,在高减排率情景下,以末端治理为主的控制措施经济可行性较差,需综合采取产业/能源结构调整、清洁生产等措施实现NO_x和VOCs的大比例减排,实现东莞O_3的稳定达标.今后将进一步研究NO_x和VOCs减排对PM_(2.5)环境浓度及健康效益影响,开展多目标污染物协同控制费效评估.     

Electrostatic forces in wind-pollination—Part 1: Measurement of the electrostatic charge on pollen

Under fair weather conditions, a weak electric field exists between negative charge induced on the surface of plants and positive charge in the air. This field is magnified around points (e.g. stigmas) and can reach values up to 3×10⁶ V m⁻¹. If wind-dispersed pollen grains are electrically charged, the electrostatic force (which is the product of the pollen's charge and the electric field at the pollen's location) could influence pollen capture. In this article, we report measurements of the electrostatic charge carried by wind-dispersed pollen grains. Pollen charge was measured using an adaptation of the Millikan oil-drop experiment for seven anemophilous plants: Acer rubrum, Cedrus atlantica, Cedrus deodara, Juniperus virginiana, Pinus taeda, Plantago lanceolata and Ulmus alata. All species had charged pollen, some were positive others negative. The distributions (number of pollen grains as a function of charge) were bipolar and roughly centered about zero although some distributions were skewed towards positive charges. Most pollen carried small amounts of charge, 0.8 fC in magnitude, on average. A few carried charges up to 40 fC. For Juniperus, pollen charges were also measured in nature and these results concurred with those found in the laboratory. For nearly all charged pollen grains, the likelihood that electrostatics influence pollen capture is evident.     

Evaluation of high volume particle sampling and sample handling protocols for ambient urban air mutagenicity determinations.

An investigation of high volume particle sampling and sample handling procedures was undertaken to evaluate variations of protocols being used by the U.S. Environmental Protection Agency. These protocols are used in urban ambient air studies which collect ambient and source samples for subsequent mutagenicity analysis of the organic extracts of the aerosol fraction. Specific protocol issues investigated include: (a) duration of sampling period, (b) type of filter media used to collect air particles, (c) necessity for cryogenic field site storage and dry ice shipping of filter samples, and (d) sample handling at the receiving laboratory. Six PM10 Hi-Vol samplers were collocated at an urban site in downtown Durham, North Carolina and operated simultaneously to evaluate 12 h versus 24 h collection periods and filter media choices of glass fiber, Teflon impregnated glass fiber (TIGF), and quartz fiber. Filters from the samplers plus field blanks were collected during each of 25 sampling periods. TIGF filters from two samplers were immediately placed on dry ice in the field and transported directly to cryogenic storage. TIGF, quartz, and glass fiber filters from three samplers were transported at ambient and maintained at room temperature for three to six days prior to cryogenic storage. One TIGF sample, which was collected on a previously tared filter, was subjected to controlled environment equilibration (40 percent relative humidity, 22 degrees C) for 8 to 24 h and weighed prior to cryogenic storage. All filters were subsequently stored at -70 degrees C to -80 degrees C prior to a one-time extraction and Salmonella (Ames) mutagenicity bioassay of the entire sample set.(ABSTRACT TRUNCATED AT 250 WORDS)