Annular Denuder System Research Articles

High-Resolution Measurements of SO2, HNO3 and HCl at the Urban Environment of Athens, Greece: Levels, Variability and Gas to Particle Partitioning

High-resolution measurements of sulfur dioxide (SO2), nitric acid (HNO3), and hydrochloric acid (HCl) were conducted in Athens, Greece, from 2014 to 2016 via a wet rotating annular denuder system paired with an ion chromatograph. Decreased mean annual levels of SO2 and HNO3 (equal to 3.3 ± 4.8 μg m−3 and 0.7 ± 0.6 μg m−3, respectively) were observed relative to the past, whereas for HCl (mean of 0.4 μg m−3 ) no such comparison was possible as the past measurements are very scarce. Regional and local emission sources regulated the SO2 levels and contributed to both the December and the July maxima of 6.6 μg m−3 and 5.5 μg m−3, respectively. Similarly, the significant enhancement at noon and during the winter nighttime was due to transported SO2 and residential heating, respectively. The oxidation of NO2 by OH radicals and the heterogeneous reactions of HNO3 on sea salt seemed to drive the HNO3 and HCl formation, respectively, whereas nighttime biomass burning affected only the former by almost 50%. During summer, the sulfate anions dominated over the SO2, in contrast to the chloride and nitrate ions that prevailed during the winter and were linked to the aerosol acidity that influences their lifetime as well as their impact on ecosystems.

Aerosol and Gas Phase Concentrations from an Adapted Annular Denuder System in a Broiler Housing Facility

HighlightsAn adapted annular denuder system (ADS) was implemented in a broiler facility to measure secondary aerosols.Results show that secondary aerosols were not always associated with ammonium or ammonia.Chloride aerosols were significant in comparison to other species and were present at consistent concentrations.This study concludes that the chloride source was the feed in the feeding pans.Abstract. Fine particulate matter (PM2.5) is present in animal housing facilities from both primary and secondary sources. Measuring secondary aerosols in harsh environments with high gas and particulate concentrations, such as poultry housing facilities, is an ongoing challenge. This study presents the results from the implementation of an adapted annular denuder system (ADS) used to measure secondary PM2.5 from inside a broiler facility in Ontario, Canada. Results from this work show that secondary aerosols formed the majority of total PM2.5 during the early portion of the growth cycle. It was further determined that the ion balance between ammonium and anions was not consistent, leading to the conclusion that a significant portion of the aerosol species are associated with a previously unidentified source that is not necessarily due to secondary reactions. Keywords: Ammonia, Annular denuder system, Particulate matter, Poultry, Secondary aerosols.

Evaluation of Alternative Annular Denuder Systems for the Collection of Fine Aerosol Particulate Matter

Due to the complex manner in which secondary inorganic aerosols (SIAs) form, a need exists to develop a methodology to measure PM2.5 emissions from agricultural operations to better understand the contribution of SIAs to the PM2.5 fraction. When sampling particulate matter (PM), annular denuder systems (ADS) are a United States Environmental Protection Agency (US EPA) approved system used to measure both gaseous and particulate components of aerosols. While collecting basic gases, such as ammonia, using nine denuders was feasibly demonstrated in poultry housing units but the ability of additional denuders to accurately collect the SIAs on the filters is yet to be demonstrated. An experiment was designed to assess particle deposition behaviors throughout three different ADS configurations. It was determined that the nine denuder configuration resulted in particles being impacted and retained, mainly in the U-bend junctions, prior to reaching the filters with only 87.2% of PM2.5 reaching the filter pack. The US EPA-prescribed ADS configuration had 99.4% of PM2.5 reaching the filters, indicating that there is an impact due to the U-Bend addition to the system. It was further demonstrated that having additional denuders in series with no U-Bend had no significant impact on PM2.5 deposition on the filters with 98.9% of PM2.5 being collected.

Isotopic characterization of nitrogen oxides (NO<sub><i>x</i></sub>), nitrous acid (HONO), and nitrate (<i>p</i>NO<sub>3</sub><sup>−</sup>) from laboratory biomass burning during FIREX

Abstract. New techniques have recently been developed and applied to capture reactive nitrogen species, including nitrogen oxides (NOx=NO+NO2), nitrous acid (HONO), nitric acid (HNO3), and particulate nitrate (pNO3-), for accurate measurement of their isotopic composition. Here, we report – for the first time – the isotopic composition of HONO from biomass burning (BB) emissions collected during the Fire Influence on Regional to Global Environments Experiment (FIREX, later evolved into FIREX-AQ) at the Missoula Fire Science Laboratory in the fall of 2016. We used our newly developed annular denuder system (ADS), which was verified to completely capture HONO associated with BB in comparison with four other high-time-resolution concentration measurement techniques, including mist chamber–ion chromatography (MC–IC), open-path Fourier transform infrared spectroscopy (OP-FTIR), cavity-enhanced spectroscopy (CES), and proton-transfer-reaction time-of-flight mass spectrometry (PTR-ToF). In 20 “stack” fires (direct emission within ∼5 s of production by the fire) that burned various biomass materials from the western US, δ15N–NOx ranges from −4.3 ‰ to +7.0 ‰, falling near the middle of the range reported in previous work. The first measurements of δ15N–HONO and δ18O–HONO in biomass burning smoke reveal a range of −5.3 ‰ to +5.8 ‰ and +5.2 ‰ to +15.2 ‰, respectively. Both HONO and NOx are sourced from N in the biomass fuel, and δ15N–HONO and δ15N–NOx are strongly correlated (R2=0.89, p<0.001), suggesting HONO is directly formed via subsequent chain reactions of NOx emitted from biomass combustion. Only 5 of 20 pNO3- samples had a sufficient amount for isotopic analysis and showed δ15N and δ18O of pNO3- ranging from −10.6 ‰ to −7.4 ‰ and +11.5 ‰ to +14.8 ‰, respectively. Our δ15N of NOx, HONO, and pNO3- ranges can serve as important biomass burning source signatures, useful for constraining emissions of these species in environmental applications. The δ18O of HONO and NO3- obtained here verify that our method is capable of determining the oxygen isotopic composition in BB plumes. The δ18O values for both of these species reflect laboratory conditions (i.e., a lack of photochemistry) and would be expected to track with the influence of different oxidation pathways in real environments. The methods used in this study will be further applied in future field studies to quantitatively track reactive nitrogen cycling in fresh and aged western US wildfire plumes.

Acid gases and aerosol measurements in the UK (1999–2015): regional distributions and trends

Abstract. The UK Acid Gases and Aerosol Monitoring Network (AGANet) was established in 1999 (12 sites, increased to 30 sites from 2006), to provide long-term national monitoring of acid gases (HNO3, SO2, HCl) and aerosol components (NO3−, SO42−, Cl−, Na+, Ca2+, Mg2+). An extension of a low-cost denuder-filter pack system (DELTA) that is used to measure NH3 and NH4+ in the UK National Ammonia Monitoring Network (NAMN) provides additional monthly speciated measurements for the AGANet. A comparison of the monthly DELTA measurement with averaged daily results from an annular denuder system showed close agreement, while the sum of HNO3 and NO3− and the sum of NH3 and NH4+ from the DELTA are also consistent with previous filter pack determination of total inorganic nitrogen and total inorganic ammonium, respectively. With the exception of SO2 and SO42−, the AGANet provides, for the first time, the UK concentration fields and seasonal cycles for each of the other measured species. The largest concentrations of HNO3, SO2, and aerosol NO3− and SO42− are found in southern and eastern England and smallest in western Scotland and Northern Ireland, whereas HCl are highest in south-eastern, south-western, and central England, that may be attributed to dual contribution from anthropogenic (coal combustion) and marine sources (reaction of sea salt with acid gases to form HCl). Na+ and Cl− are spatially correlated, with largest concentrations at coastal sites, reflecting a contribution from sea salt. Temporally, peak concentrations in HNO3 occurred in late winter and early spring attributed to photochemical processes. NO3− and SO42− have a spring maxima that coincides with the peak in concentrations of NH3 and NH4+, and are therefore likely attributable to formation of NH4NO3 and (NH4)2SO4 from reaction with higher concentrations of NH3 in spring. By contrast, peak concentrations of SO2, Na+, and Cl− during winter are consistent with combustion sources for SO2 and marine sources in winter for sea salt aerosol. Key pollutant events were captured by the AGANet. In 2003, a spring episode with elevated concentrations of HNO3 and NO3− was driven by meteorology and transboundary transport of NH4NO3 from Europe. A second, but smaller episode occurred in September 2014, with elevated concentrations of SO2, HNO3, SO42−, NO3−, and NH4+ that was shown to be from the Icelandic Holuhraun volcanic eruptions. Since 1999, AGANet has shown substantial decrease in SO2 concentrations relative to HNO3 and NH3, consistent with estimated decline in UK emissions. At the same time, large reductions and changes in the aerosol components provide evidence of a shift in the particulate phase from (NH4)2SO4 to NH4NO3. The potential for NH4NO3 to release NH3 and HNO3 in warm weather, together with the surfeit of NH3 also means that a larger fraction of the reduced and oxidized N is remaining in the gas phase as NH3 and HNO3 as indicated by the increasing trend in ratios of NH3 : NH4+ and HNO3 : NO3− over the 16-year period. Due to different removal rates of the component species by wet and dry deposition, this change is expected to affect spatial patterns of pollutant deposition with consequences for sensitive habitats with exceedance of critical loads of acidity and eutrophication. The changes are also relevant for human health effects assessment, particularly in urban areas as NH4NO3 constitutes a significant fraction of fine particulate matter ( < 2.5 µm) that are linked to increased mortality from respiratory and cardiopulmonary diseases.

Collection Method for Isotopic Analysis of Gaseous Nitrous Acid.

The sources and chemistry of gaseous nitrous acid (HONO) in the environment are of great interest. HONO is a major source of atmospheric hydroxyl radical (OH), which impacts air quality and climate. HONO is also a major indoor pollutant that threatens human health. However, the large uncertainty of HONO sources and chemistry hinders an accurate prediction of the OH budget. Isotopic analysis of HONO may provide a tool for tracking the sources and chemistry of HONO. In this study, a modified annular denuder system (ADS) was developed to quantitatively capture HONO for offline nitrogen and oxygen isotopic analysis (δ15N and δ18O) using the denitrifier method. The ADS method was tested using laboratory generated HONO (400 ppbv to 1 ppmv) and validated by parallel HONO collection with a standard, basic impinger (BI) method. The ADS system shows complete capture of HONO without isotopic fractionation. The uncertainty (1σ) based on repeated measurements across the entire analytical procedure is 0.6‰ for δ15N and 0.5‰ for δ18O. The ADS method was also tested in roadside collections of ambient HONO (0.4-1.3 ppbv) for isotopic analysis and was found to be robust for low concentration collections over 3 and 12 h collection times. In order to ensure ability to use this method in the laboratory and in the field, storage conditions for the collected HONO samples were tested and samples can be stored with consistent δ15N and δ18O for 60 days. This method enables future work to utilize the isotopic composition of HONO for studying HONO chemical formation pathways, as well as atmospheric sources and chemistry.

Field performance of a semi-continuous monitor for ambient PM2.5 water-soluble inorganic ions and gases at a suburban site

To reduce sampling artifacts and to improve time-resolved measurements of inorganic aerosol system, a recently commercialized semi-continuous In-situ Gas and Aerosol Composition (IGAC) monitoring system was evaluated against a reference annular denuder system (ADS; denuder/two-stage filter pack) at a suburban site over a year, during which the average PM2.5 was 37.0 ± 24.8 μg/m3. A suite of eight ions SO42−, NO3−, Cl−, NH4+, Na+, K+, Ca2+ and Mg2+ and two gases SO2 and NH3 were the target species. In comparison to the reference ADS method, the IGAC performed well in measuring the major ions SO42−, NO3− and NH4+, and the SO2. For those species, the linear slopes, intercepts and R2 values between the two methods all passed the performance evaluation criteria outlined by earlier similar studies. The performance of IGAC on Cl−, Na+, K+ and NH3 was marginally acceptable, whereas Ca2+ and Mg2+ could not be properly evaluated due to the low concentrations (<0.2 μg/m3) and hence inadequate amount of sample size. The ionic balance of the hourly IGAC samples averaged very close to unity, as did the daily ADS samples, though the former was considerably more variable than the latter. The overall performance of the IGAC has been shown to be comparable to other similar monitors and its improvements are discussed.

Comparison of NO2 and SO2 Measurements Using Different Passive Samplers in Tropical Environment

This report describes the results of an inter-comparison study conducted for the sampling and analysis of NO2 and SO2 by using different type of passive samplers in tropical urban environment. For this purpose, field experiments were proposed to be conducted by two round robin tests from Sept. 2007 to Aug. 2008 in Singapore. A set of different types of passive samplers have been exposed to ambient air at atmospheric research station in National University of Singapore along with suitable active samplers (as reference method) for a sufficient period of time (3–4 weeks). Annular denuder system (ADS) active sampling data showed that NO2 concentration level (23.8–28.1 ppb) in Singapore was slightly higher than the WHO guideline but SO2 concentration (12.5–14.9 ppb) was approximately twice the value of WHO guideline. For the two round robin tests, accuracy analysis by using active sampling data as reference demonstrated that grand mean values from passive air sampling (PAS) and active sampler average concentrations, for both NO2 and SO2, are in close agreement with each other. Precision evaluation based on the triplicate samplers co-located at the same sampling site Singapore showed that most of the passive samplers applied here had repeatability. ANOVA statistical analysis also showed no significant difference between the measurement data obtained by different type of passive samplers for both round robin tests in Singapore.

Size mass distribution of water-soluble ionic species and gas conversion to sulfate and nitrate in particulate matter in southern Taiwan

A Micro-Orifice Uniform Deposition Impactor (MOUDI) and a Nano-MOUDI were employed to determine the size-segregated mass distributions of ambient particulate matter (PM) and water-soluble ionic species for particulate constituents. In addition, gas precursors, including HCl, HONO, HNO3, SO2, and NH3 gases, were analyzed by an annular denuder system. PM size mass distribution, mass concentration, and ionic species concentration were measured during the day and at night during episode and non-episode periods in winter and summer. Average total suspended particle (TSP) concentrations during episode days in winter were as high as 153 ± 33 μg/m(3), and PM mass concentrations in summer were as low as one-third of that in winter. Generally, PM concentration at night was higher than that in the daytime in southern Taiwan during the sampling periods. In winter during the episode periods, the size-segregated mass distribution of PM mass concentration was mostly in the 0.32-3.2-μm range, and the PM concentration increased significantly in the range of 0.32-3.2 μm at night. Ammonium, nitrate, and sulfate were the dominant water-soluble ionic species in PM, contributing 34-48% of TSP mass. High concentrations of ammonia (12.9-49 μg/m(3)) and SO2 (2.6-27 μg/m(3)) were observed in the gas precursors. The conversion ratio was high in the PM size range of 0.18-3.2 μm both during the day and at night in winter, and the conversion ratio of episode days was 20% higher than that of non-episode days. The conversion factor was high for both nitrogen and sulfur species at nighttime, especially on episode days.

Evaluation of an annular denuder system for carbonaceous aerosol sampling of diesel engine emissions

Sampling of particle-phase organic carbon (OC) from diesel engines is complicated by adsorption and evaporation of semivolatile organic carbon (SVOC), defined as positive and negative artifacts, respectively. In order to explore these artifacts, an integrated organic gas and particle sampler (IOGAPS) was applied, in which an XAD-coated multichannel annular denuder was placed upstream to remove the gas-phase SVOC and two downstream sorbent-impregnated filters (SIFs) were employed to capture the evaporated SVOC. Positive artifacts can be reduced by using a denuder, but particle loss also occurs. This paper investigates the IOGAPS with respect to particle loss, denuder efficiency, and particle-phase OC artifacts by comparing OC, elemental carbon (EC), SVOC, and selected organic species, as well as particle size distributions. Compared to the filter pack methods typically used, the IOGAPS approach results in estimation of both positive and negative artifacts, especially the negative artifact. The positive and negative artifacts were 190 µg/m3 and 67 µg/m3, representing 122% and 43% of the total particle OC measured by the IOGAPS, respectively. However, particle loss and denuder break-through were also found to exist. Monitoring particle mass loss by particle number or EC concentration yielded similar results ranging from 10% to 24% depending upon flow rate. Using the measurements of selected particle-phase organic species to infer particle loss resulted in larger estimates, on the order of 32%. The denuder collection efficiency for SVOCs at 74 L/min was found to be less than 100%, with an average of 84%. In addition to these uncertainties the IOGAPS method requires a considerable amount of extra effort to apply. These disadvantages must be weighed against the benefits of being able to estimate positive artifacts and correct, with some uncertainty, for the negative artifacts when selecting a method for sampling diesel emissions. Implications: Measurements of diesel emissions are necessary to understand their adverse impacts. Much of the emissions is organic carbon covering a range of volatilities, complicating determination of the particle fraction because of sampling artifacts. In this paper an approach to quantify artifacts is evaluated for a diesel engine. This showed that 63% of the particle organic carbon typically measured could be the positive artifact while the negative artifact is about one-third of this value. However, this approach adds time and expense and leads to other uncertainties, implying that effort is needed to develop methods to accurately measure diesel emissions. Supplemental Materials: Supplemental materials are available for this paper. Go to the publisher's online edition of the Journal of the Air & Waste Management System.

Characteristics of Nitrogenous Air Pollutants at Urban and Suburban Forested Sites, Western Japan

Nitrogenous air pollutants including nitrogen dioxide (NO2), nitric acid (HNO3), nitrate (NO 3 − ), ammonia (NH3), ammonium (NH 4 + ), and nitrous acid (HONO) were characterized at an urban forested (UF) site in Hiroshima and at a suburban forested (SF) site in Fukuoka, western Japan, using an annular denuder system for 1 year from May 2006 to May 2007 to compare the concentrations and chemical species of atmospheric nitrogenous pollutants between UF and SF sites. The proximity of the urban area was reflected in higher NO2 concentrations at the UF site than at the SF site. NO2 was more oxidized at the SF site because it is farther from an urban area than the UF site, which was reflected in higher concentrations of HNO3 at the SF site than the UF site. HNO3 and acidic sulfate is neutralized by NH3, existing as ammonium nitrate (NH4NO3) and ammonium sulfate [(NH4)2SO4] at the UF site. At the SF site, acidic sulfate is neutralized by NH3, existing as (NH4)2SO4, but NH4NO3, had scarcely formed at the SF site. A much higher HONO concentration was observed at the UF site than at the SF site, especially in winter and spring at night, which could be explained by higher NO2 concentrations at the UF site because of its proximity to an urban area and stagnant meteorological conditions. Atmospheric HONO determination was critical in evaluating the possibility of damage to trees in UF areas.

Ambient ammonia in terrestrial ecosystems: A comparative study in the Tennessee Valley, USA

Atmospheric ammonia has been shown to degrade regional air quality and affect environmental health. In-situ measurements of ammonia are needed to determine how ambient concentrations vary in different ecosystems and the extent to which emission sources contribute to those levels. The objective of this study was to measure and compare ammonia concentrations in two Tennessee Valley (USA) ecosystems: a forested rural area and a metropolitan site adjacent to a main transportation route. Integrated samples of atmospheric ammonia were collected with annular denuder systems for ~ 4 weeks during the summer of 2009 in both ecosystems. Ancillary measurements of meteorological variables, such as wind direction and precipitation, were also conducted to determine any relationships with ammonia concentration. Measurements in the two ecosystems revealed ammonia concentrations that were mostly representative of background levels. Arithmetic means were 1.57 ± 0.68 μg m − 3 at the metropolitan site and 1.60 ± 0.77 μg m − 3 in the forest. The geometric mean concentrations for both sites were ~ 1.46 μg m − 3 . Wind direction, and to a lesser extent air temperature and precipitation, did influence measured concentrations. At the metropolitan site, ammonia concentrations were slightly higher in winds emanating from the direction of the interstate highway. Meteorological variables, such as wind direction, and physical factors, such as topography, can affect measurement of ambient ammonia concentrations, especially in ecosystems distant from strong emission sources. The 12-h integrated sampling method used in this study was unable to measure frequent changes in ambient ammonia concentrations and illustrates the need for measurements with higher temporal resolution, at least ~ 1–2 h, in a variety of diverse ecosystems to determine the behavior of atmospheric ammonia and its environmental effects.

An annular denuder system for the collection of elevated quantities of ammonia to allow for the measurement of inorganic reactive gases and aerosol species inside poultry houses

The annular denuder system (ADS) is an instrument for trapping and subsequently analysing for concentrations of inorganic reactive gases and aerosol species in the atmosphere. Todate its application in the livestock industry is limited primarily by its inability to collect gaseous ammonia at the elevated levels commonly observed in livestock operations. The study’s objective was to improve upon the ammonia collection capabilities of the ADS to determine if it was potentially suitable for in-house sampling. Using a 1% phosphorous acid coating, a single denuder becomes less than 100% efficient at collecting gaseous ammonia after 0.65 mg of ammonia was absorbed on the denuder’s walls. The loading capacity of the denuder was determined to be 2.39 ± 0.23 mg of ammonia. Ammonia saturation problems were alleviated by using seven denuders in series to collect a representative ammonia level (25 ppm) for poultry facilities over an hour sampling period. The extended ADS was calibrated against three ammonia gas standards and an ammonia monitor. The mean error was determined to be 2.39% using the ammonia standards and it was within 5.1%, on average, of the ammonia measurements using the continuous ammonia monitor inside a layer facility.

Causes of the elevated nitrate aerosol levels during episodic days in Taichung urban area, Taiwan

The purpose of this study is to explore the possible reasons accounting for elevated nitrate aerosol levels during high particulate days (HPD) in Taichung urban area of central Taiwan. To achieve this goal, simultaneous measurements of particulate and gaseous pollutants were carried out from September 2004 to April 2005 using an annular denuder system (ADS). The formation rate of NO 2 to nitrate aerosol, calculated using the relevant chemical reactions, was employed to interpret enhanced nitrate aerosol concentrations during HPD. The observations showed that nitrate concentration during HPD was 14 times higher than that during low particulate days (LPD). The average formation rate during HPD was 4.0% h −1, which was 3.1 times higher than that during LPD. The quantitative analysis showed that the formation rate was mainly influenced by temperature and relative humidity. Lower temperature and higher relative humidity led much nitrate aerosol formation in HPD. Moreover, the residence time analysis of air masses staying over the studied area showed that the slow-motion air retained high nitrate concentrations due to more nitrate aerosol converted from the precursors in NOx-rich areas.

Characteristics of atmospheric nitrogen and sulfur containing compounds in an inland suburban-forested site in northern Kyushu, western Japan

To evaluate the effects of the regional pollutant emission and long-range transport from East Asia of nitrogen and sulfur pollutants on air quality at an inland suburban-forested site in northern Kyushu, western Japan, nitrogen and sulfur pollutants were characterized from May 2006 to April 2007 using an annular denuder system. The annual mean concentration of HNO 3 (2.16 μg m − 3 ) at the study site was comparable to concentrations reported in urban areas. The HNO 3 concentration had a diurnal variation, being higher in daytime and lower at night. The diurnal variation of wind direction suggests air pollutants emitted from the regional urban area were transported to the study site during the daytime and caused a higher HNO 3 concentration. The HNO 3 concentration was significantly higher in summer and spring than in winter. The annual mean concentrations of SO 2 and nss-SO 4 2− (6.52 and 7.70 μg m − 3 , respectively) were higher than concentrations determined in other urban areas and forested areas near urban areas in Japan and other countries. The SO 2 concentration was significantly higher in winter and spring than in summer. Backward trajectory analysis indicates the long-range transport from East Asia partly contributed to the higher concentrations of SO 2 in winter and spring. In contrast, there were no statistical differences in the nss-SO 4 2− concentrations among seasons, which could be explained by increased oxidation of SO 2 to SO 4 2− in summer. The value of sulfur conversion ratio ( F s) being higher throughout the year at the study site (52.6%) than values determined in urban sites and there being no diurnal variation of F s indicates the long-range transport of nss-SO 4 2− not only from East Asia but also from other areas including Japan. The equivalent ratio of NH 4 + and nss-SO 4 2− at the study site (0.96 ± 0.22) indicates that acidic sulfate is neutralized by NH 3, existing mainly as (NH 4) 2SO 4 in fine particles. On the other hand, NH 4NO 3 had scarcely formed at the study site, unlike the case for urban areas. Ca 2+ and Na + are suggested to be the counter ions of NO 3 − in coarse particles, which is similar to the situation for the sites where the concentration of NH 3 is insufficient for NH 4NO 3 to form.

Spatial variability of sulfur dioxide and sulfate over complex terrain in East Tennessee, USA

In 2004 and 2005, the East Tennessee Ozone Study (ETOS) enhanced its regional measurement program with annular denuder systems to quantify sulfur dioxide (SO 2) and PM 2.5 sulfate (SO 4 2−) at five sampling sites that were representative of the complex terrain and physiographic features of East Tennessee. Intersite spatial variability was more defined for SO 2 than for SO 4 2−, which showed a fairly uniform structure in both daytime and nighttime measurements. Pollution roses indicated that two sites may have been influenced by the proximity of SO 2 emission sources. The data suggest that SO 2 is affected by nearby sources in the study area while the sources of SO 4 2− are regionally distributed.

Assessing the Relationship between Air Mass Age and Summer Ozone Episodes Based on Photochemical Indices

Although pollutant sources are usually in urban and industrialized areas, poor air quality is frequently encountered in downwind rural areas. This study utilized a tethered balloon to measure the pollutant concentrations in a downwind side (Caotun) of the Taichung Basin during the summer of 2002. Furthermore, an annular denuder system (ADS) was used to measure PM2.5 and gaseous pollutant concentrations. Concentrations of 55 VOCs species were measured continuously by a network of photochemical assessment monitoring stations in central Taiwan. This study discusses the correlation between the ozone concentration and the routes of an air mass during ozone episodes. Backward trajectory, ratio of particulate matter and photochemical indices were used to examine the aging degree of an air mass. During ozone episodes, the trajectory distribution had a clear sea-land breeze mechanism with a relatively slow wind speed, and the air mass primarily entered through the western coastal industrial area. Analytical results demonstrate that daytime ozone concentrations accompany HNO3 concentrations by photochemical reactions and depend on the previous night’s HNO2 concentration. The sulfur and nitrogen conversion ratios, and the photochemical indices (ethylbenzene/m,p-xylene, n-pentane/t-2-pentene and NO2/NO) increased with the ozone concentration. The downwind photochemical indices were strongly correlated with ozone concentration and were higher than those upwind. These phenomena indicate that the air mass during ozone episodes belongs to the “more aged” category.

미세입자(PM2.5)의 질산염 (NO3-) 휘발 특성 분석 -서울시 4개 측정지역을 중심으로-

The purpose of this study is to understand the impact that temperature and relative humidity have on the volatilization loss of particulate nitrate <TEX>$(NO_3^-)$</TEX> from Teflon filters during measurements of ambient fine particles <TEX>$(PM_{2.5})$</TEX>. Fine particles <TEX>$(d_p</TEX><TEX><</TEX><TEX>2.5{\mu}m)$</TEX> were measured using an annular denuder system (ADS) at four representive areas in Seoul. The measurements were made during 28 different days at 24-hr sampling intervals from February 14 to October 15, 1997. In this study, nitrate losses. calculated by the ratio of nitrate on the nylon filter to their sum in both Teflon and nylon titters, varied seasonally in the following order: summer (45.5%) > spring (23.8%) > fall (20.6%) > winter (19.7%). The results showed strong correlations with temperature, but we did not observe any significant effects of relative humidity. However, we observed that both temperature and relative humidity influenced the ambient gas/particle nitrate ratio in a different case study using a denuder.

Concentrations and Formation Rates of Ambient Nitrous Acid in Taichung City, Taiwan

This paper investigates the concentrations and formation rates of ambient nitrous acid (HNO2) in the urban atmosphere. Simultaneous measurements of HNO2 and aerosol particles were carried out from July 2005 to January 2006 by using an annular denuder system (ADS). In addition, the formation rates of NOx to HNO2 were assessed by evaluating potential reactions. The HNO2 concentrations ranged from 0.1 to 15.3 μg m−3 with a mean value of 2.9 μg m−3. The lower levels of HNO2 found in the 10–14 and 14–18-h sampling intervals were due to photolytic reactions. Moreover, heterogeneous reactions of NO2 and H2O on the aerosol surface contributed to the numerous production pathways of HNO2 during nighttime, which was verified by experimental observations and theoretical evaluations. The formation rates of HNO2 ranged from 0.5–2.6 % h−1, while the highest values were found at nighttime. Finally, the factors affecting the formation rate were investigated using sensitivity analysis. The results showed that HNO2 was sign...

Gaseous and aerosol pollutants during fog and clear episodes in South Asian urban atmosphere

We report the first measurements of acidic gases and ammonia (NH 3) during fog and clear episodes in Lahore, a highly polluted mega-city of South Asia, along with concentrations of PM 2.5 (particles of <2.5 μm aerodynamic diameter) and ions. An annular denuder system was used to measure acidic gases, NH 3, and PM 2.5 from December 2005 to February 2006 in Lahore, a mega-city in Pakistan. The denuders yielded average concentrations (μg m −3) as follows: ammonia, 50; nitrous acid, 19.6; sulfur dioxide, 19.4; hydrochloric acid, 1.16; nitric acid, 1.00; and oxalic acid, 0.6. The filters yielded average concentrations (μg m −3): PM 2.5, 209; sulfate, 19.2; nitrate, 18.9; chloride, 7.43; oxalate, 0.97; ammonium, 16.1; potassium, 3.49; calcium, 0.89; sodium, 0.76; and magnesium, 0.08. Emissions from local sources, e.g., fossil fuel consumption by motorized transport and power plants, farming, burning of agricultural residues, industrial and construction activities contributed the major proportion of pollutants in Lahore. Concentrations of ionic species, e.g., NO 3 −, SO 4 2−, Na +, NH 4 +, Mg 2+, and Ca 2+, and gaseous species, e.g., HCl, HNO 3, SO 2 and (COOH) 2 showed a distinct diurnal variation. Mixing heights and photochemistry played major roles in defining the diurnal pattern. Fog appeared to profoundly enhance the oxidation of sulfur dioxide. High moisture content of fog resulted in uptake of the gases in fog droplets.