Characterization of atmospheric trace elements on PM2.5 particulate matter over the New York–New Jersey harbor estuary

The purpose of this work is to characterize trace elements associated with atmospheric particulate matter of 2.5 μm and smaller in size (PM_2.5) over the New York–New Jersey (NY–NJ) Harbor Bight. Using low-volume PM_2.5 samplers, aerosol particulate samples were simultaneously collected for the first time at three locations in the region, Sandy Hook in the coast, New Brunswick and Liberty Science Center (Jersey City) in nearby urban areas, during January 1998–January 1999. Sample analysis for trace elements was accomplished by inductively coupled plasma mass spectrometry. Many elements in ambient air exhibit strong spatial gradients from urban centers to the coast, and the concentrations of most elements at Liberty Science Center are significantly higher than at the other two locations. Seasonal patterns are not apparent for most elements at all locations, suggesting continuous contributions from their sources. The elements Pb, Cd, Zn, Cu, Ni, V, Sb, are enriched by factors of 200 to 20,000 relative to their natural abundance in crustal soil. Major sources that contribute to the atmospheric loading of these elements include fossil fuel combustion, oil combustion, metal processing industry, and waste incineration. Atmospheric dry deposition of these trace elements associated with PM_2.5 to the coastal waters of the NY–NJ estuary may account for a significant portion of the total dry deposition fluxes for these elements.     

Bio- and toxic elements in mushrooms from the city of Umeå and outskirts,Sweden

Edible mushrooms (Albatrellus ovinus, Boletus edulis, Clitocybe odora, Gomphidius glutinosus, Leccinum scabrum, Leccinum versipelle, Lycoperdon perlatum, Suillus bovinus, Suillus luteus, and Xerocomus subtomentosus) collected from unpolluted areas of the city of Umeå and its outskirts in the northern part of Sweden were examined for contents of toxic metallic elements (Cd, Pb, and Ag) and essential macro- and microelements (K, Na, Ca, Mg, Cu, Fe, Mn, and Zn) using a validated method and a final measurement by flame atomic absorption spectroscopy (F-AAS). The median values of the toxic metallic element concentrations (in mg kg^?1 dry biomass, db) ranged from: 0.12–3.9, 0.46–5.1, and 0.91–6.2 for Ag, Cd and Pb, respectively. For the essential metallic elements, the median values of concentrations ranged from: 24000–58000, 15–2000, 59–610, 520–1900, 2.0–97, 16–150, 15–120, and 4.3–26 mg kg^?1 db for K, Na, Ca, Mg, Cu, Zn, Fe, and Mn, respectively. The baseline concentrations of the metallic elements determined in mushrooms were mainly affected by the fungal species. The assessed probable maximal dietary intake of Cd (0.002 mg kg^?1 body mass) solely from a mushroom meal was only slightly below a revised value of the tolerable weekly intake for this element, while for Pb (0.003 mg kg^?1 body mass) it was tenfold below the provisionally tolerable weekly intake.     

Changes in the wet precipitation of sodium and chloride over the continental United States, 1984–2006

Data on wet-only precipitation from the National Atmospheric Deposition Program/National Trends Network were analysed for trends in the sodium and chloride fluxes over the United States between 1 January 1984 and 31 December 2006. The data were first checked for consistency and for ionic balance. It was necessary to correct for changes in bicarbonate due to changes in atmospheric CO₂ levels over the study period, in order to obtain a balance. The fluxes were calculated and the trends determined by linear regression in the log domain. The significance of the trends was checked using both F- and t-tests. At 154 sites having reasonably continuous records over the assessment period, the sodium flux fell significantly at 139 and increased significantly at only one. The chloride flux similarly fell significantly at 140 and increased significantly at the same one as the sodium flux increased. At coastal sites the chloride to sodium ratio was the same as that in sea water, within experimental limits. Further from the coast the ratio changed apparently due to changes in the entire aerosol chemistry. The findings are discussed in terms of the simplicity and robustness of the methodology employed to determine the trends; the oceanic origin of most observable sodium even in the interior of the continent, probably because it occurs as a fine (<1 micron) aerosol which is poorly scavenged by precipitation; and the possibility that the drop in sodium and chloride fluxes might be driven by climate change.     

Coarse–fine and day–night differences of water-soluble ions in atmospheric aerosols collected in Christchurch and Auckland,New Zealand

The water-soluble ions in fine (PM_<2.5) and coarse (PM_2.5−10) atmospheric aerosols collected in Christchurch during winter 2001, spring 2000 and summer 2001, and in Auckland during winter 2001 have been studied in terms of coarse–fine and day–night differences. Although the chemical characteristics of the coarse particles were similar in both cities, those of the fine particles collected in the Christchurch winter were significantly different, as manifested by higher concentrations of nss-K⁺, nss-Cl⁻, nss-Ca²⁺, nss-SO₄²⁻, NO₃⁻ and NH₄⁺. It was found that nighttime PM₁₀ and nss-K⁺ concentrations were much higher than their daytime concentrations in the Christchurch winter but a clear day–night difference was not apparent in the Auckland winter. Moreover, in the winter, sea-salt ions did not show a day–night difference; however, nss-SO₄²⁻ had opposite day–night variation in the two cities. An ion balance calculation has shown that in most samples, coarse particles can be neutral or alkaline, however, fine particles can be neutral or acidic. The possibility of ammonium salts existing in the fine particles collected in the Christchurch winter is discussed and it is concluded that a variety of ammonium salts were present. Equivalent ratios suggest that the fine particles may be significantly aged in the Christchurch winter.The evidence from our soluble ion study strongly suggests that wood and coal burning and secondary aerosols make a significant contribution to fine particulate mass in the Christchurch atmosphere. Thus, home-heating, a sheltered geographic location and relatively calm atmospheric condition are thought to be the major causes for the serious atmospheric particulate pollution in the Christchurch winter.     

Measurement of plutonium isotopes, 239Pu and 240Pu,in air-filter samples from Seville (2001–2002)

Since the last nuclear atmospheric test carried out by the People Republic of China in 1980 and since the Chernobyl accident in 1986, the plutonium hasn't been directly released into the atmosphere. However, nowadays, it is still present in the troposphere. This is due to plutonium-bearing soil particles physical resuspension processes. In this work, we study for the first time the temporal variation of plutonium isotopes, ²³⁹Pu and ²⁴⁰Pu, baseline concentrations on a monthly basis in surface air from Seville (Spain), and their correlation with some tracers of mineral dust, during 2001 and 2002. The Pu analyses were performed by low-energy Accelerator Mass Spectrometry (AMS). The ²³⁹Pu plus ²⁴⁰Pu (^239+240Pu) activity levels achieved maximums during the summer period, characterized by the absence of rains, and minimums during the rainy seasons, laying in the range 1–20 nBq m^?3. The ²⁴⁰Pu/²³⁹Pu two-year average atomic ratio was 0.18 ± 0.03, in agreement with the fallout plutonium. A good correlation with Pu and Al and Ti levels is observed. They are crustal components usually used as tracers of African dust over European countries. The hypothesis of the influence of the Saharan dust intrusions is supported as well through the study of Total Ozone Mass Spectrometer (TOMS) daily images.     

Characteristics of lead geochemistry and the mobility of Pb isotopes in the system of pedogenic rock–pedosphere–irrigated riverwater–cereal–atmosphere from the Yangtze River delta region,China

Knowledge of the characteristics of Pb and its isotopic transfer in different compartments is scant, especially for the mobility of Pb isotopes in the geochemical cycle. The present study characterizes differential Pb transport mechanism and the mobility of Pb isotopes in the pedogenic parent rock–pedosphere–irrigated riverwater–cereal–atmosphere system in the Yangtze River delta region, by determining Pb concentration and Pb isotopic ratios of pedogenic parent rocks, fluvial suspended particle matter, tillage soils, soil profiles, irrigated riverwater, fertilizer, Pb ore, cereal roots and grains. The results show that Pb isotopes in the geochemical cycle generally follow the equation of ²⁰⁸Pb/²⁰⁶Pb = −1.157 × ²⁰⁶Pb/²⁰⁷Pb + 3.46 (r² = 0.941). However, Pb isotopes have different mobility in different environmental matrixes. Whereas in the pedosphere, the heavier Pb (²⁰⁸Pb) usually shows stronger mobility relative to the lighter Pb, and is more likely to transfer into soil exchangeable Pb fraction and carbonates phase. The lighter Pb shows stronger transfer ability from soil to cereal grain via root compared to the heavier Pb. However, the cereal grains have lower ²⁰⁶Pb/²⁰⁷Pb and higher ²⁰⁸Pb/²⁰⁶Pb ratios than root and tillage soil, similar to the airborne Pb and anthropogenic Pb, implying that a considerable amount of Pb in cereal grains comes from the atmosphere. The estimate model shows that 16.7–52.6% (average: 33.5%) of Pb in rice grain is the airborne Pb.     

An hypothesis describing the general temporal and spatial distribution of alfresco bacteria in the earth’s atmospheric surface layer

An hypothesis is presented that describes, in general terms, the temporal and spatial airborne bacterial distribution patterns in the mixed layer of the planetary atmosphere. It is hypothesized that the near coincidence of the solar radiation cycle and temporal atmospheric bacterial distribution patterns indicate that the bacterial distribution in the alfresco atmosphere is a function of the diurnal and annual solar cycles. A maximum concentration of bacteria is found in reference to the solar zenith as a standing wave in the rotating coordinate system of the moving earth. Conditions of weather, topography, source strength, and human activities (i.e. microbial air pollution-MAP) will modulate the cyclic patterns of atmospheric bacterial loadings.     

Spatiotemporal distribution and short-term trends of particulate matter concentration over China, 2006–2010

Air quality problems caused by atmospheric particulate have drawn broad public concern in the global scope. In the paper, the spatiotemporal distributions of fine particle (PM2.5) and inhalable particle (PM10) concentrations estimated with the artificial neural network (ANN) over China during 2006 to 2010 have been discussed. Most high PM10 concentration appears in Xinjiang, Qinghai, Gansu, Ningxia, Hubei, and parts of Inner Mongolia. The distribution of PM2.5 concentration is consistent with China’s three gradient terrains. The seasonal variations of PM2.5 and PM10 concentrations both indicate that they are higher in north China in spring and winter, lowest in summer. In autumn, most provinces in south China appear high value. In particular, high PM2.5 concentration appears in the southeast coastal cities while high PM10 concentration prefers the central regions in south China. On this basis, seasonal Mann–Kendall test method is utilized to analyze the short-term trends. The results also show significant changes of PM2.5 and PM10 concentrations of China in the past 5 years, and most provinces present the tendency of reduction (3–5 μg/m³ for PM2.5 and 10–20 μg/m³ for PM10 per year) while a fraction of provinces appear the increasing trend of 8–16 μg/m³ (PM2.5) and 16–30 μg/m³ (PM10). Simultaneously, PM2.5 population exposure is discussed with the combination of population density-gridded data. Municipalities get much higher exposure level than other provinces. Shanghai suffers the highest population exposure to PM2.5, followed by Beijing and then Tianjin, Jiangsu province. Most provincial capitals, such as Guangzhou, Nanjing, Chengdu, and Wuhan, face much higher exposure level than other regions of their province. Moreover, the PM2.5 exposure situation is more serious in southeast than northwest regions for Beijing-Tianjin-Hebei region. Also, per capita PM2.5 concentration and population-weighted PM2.5 concentration are calculated. The former shows that the high-level regions distribute in Guangdong, Shanghai, and Tianjin, while the latter in Hebei, Chongqing, and Shandong provinces. Further studies may consider optimizing concentration estimation model and use it to discuss the effects of particulate matters on human health.     

Study on ambient concentrations of PM10, PM10–2.5, PM2.5 and gaseous pollutants. Trace elements and chemical speciation of atmospheric particulates

This study provides the first comprehensive report on mass concentrations of particulate matter of various sizes, inorganic and organic gas concentrations monitored at three sampling sites in the city of Palermo (Sicily, Italy). It also provides information on the water-soluble species and trace elements. A total of 2054 PM₁₀ (1333) and PM_2.5 (721) daily measurements were collected from November 2006 to February 2008. The highest mass concentrations were observed at the urban stations, average values being about two times higher than those at the suburban (control) site. Time variations in PM₁₀ and also PM_10–2.5 were observed at the urban stations, the highest concentrations being measured in autumn and winter. CO, NOx, NO₂, benzene, toluene and o-xylene concentrations peaked in autumn and winter, a pattern similar to those recorded for PM₁₀ and PM_10–2.5 mass levels, indicating the importance of traffic emissions in urban air pollution. 91% and 51% of the benzene measurements exceeded the limit of 5 μg m^?3 at the two urban monitoring sites. Trace elements (As, Ba, Cr, Cu, Mo, Pb, Sb) suspected of being introduced into the atmosphere mainly by anthropogenic activities, were highly enriched with respect to local soil. Results indicate that a large fraction of PM₁₀ (31–47% in weight) and PM_2.5 (29% in weight) is made up of water-soluble ions. Ammonium sulphate and nitrate particles accounted for 14–29 wt% of particulate matter mass concentrations. Crustal and marine components, combined, account for 41% and 49% in PM_2.5 and PM₁₀, respectively. The calculated deficits in Cl^- and NH₄⁺ ions suggest that a proportion of these ions are lost, via the formation of gaseous NH₄Cl or HCl and NH₃.     

Analysis of essential and non-essential trace elements in the organs of a mother–fetus pair of spotted seals (Phoca largha) from the Sea of Japan

Environmental Science and Pollution Research - Concentrations of 22 essential and non-essential trace elements (Be, Al, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, As, Se, Mo, Ag, Cd, Sb, Ba, Tl, Pb, Th, U, and...     

Measurements of CCl3F and CCl4 at harwell over the period January 1975–June 1981 and the atmospheric lifetime of CCl3F

Measurements of CCl₃F and CCl₄ in the ambient air have been made at Harwell since October 1974. The background CCl₃F concentration at Harwell has increased with time throughout the period up to June 1981 when it had reached a value of 191 ppt. The increase was about 1.1 ppt month⁻¹ at the start of our study but it has now slowed down following the levelling off in global CCl₃F emissions. This data set represents one of the longest maintained attempts to determine the growth in CCl₃F in which careful attention has been paid to details of absolute calibration. Over the period that the measurements have been made the CCl₃F concentration has increased by over a half its original value, which provides a solid basis for comparison with release estimates.Two dimensional modelling is employed to obtain the atmospheric lifetime of CCl₃F from the observed Harwell 1975–1981 times series and the published CCl₃F historical release. The “best estimate” of the CCl₃F atmospheric lifetime is 75 y with 5–95 % confidence limits of 65–90 y. The limits are much tighter than those obtained from the first 3 y of data which would in principle have allowed a lifetime as short as 18 y (Penkett et al., 1979). This latest estimate of 75 y is wholly consistent with current theoretical estimates of the atmospheric lifetime due to stratospheric photolysis alone.Since 1979 the precision and resolution of the CCl₄ measurements at Harwell has been significantly improved. The background CCl₄ concentration found at Harwell for 1980–1981 is found to be 99–102 ppt. Whilst these values are in excellent agreement with model calculations assuming CCl₄ is wholly man-made in origin they are somewhat lower than some other published observations. Simultaneous observations of elevated concentrations of CCl₃ F and CCl₄ support the contention that CCl₄ is largely of man-made origins.     

Trends and Variability of Ground-Level O3 in Connecticut over the Period 1981–1997

Abstract

The temporal and spatial characteristics of ground-level (tropospheric) O₃ measured at 10 monitoring stations in Connecticut were studied from 1981 to 1997. To detect the O₃ trend caused by changes in precursor emissions, moving average filters and a linear least-squared regression model were used to eliminate the short-term variation and effects of temperature from raw time-series O₃ data. The results showed a significant decrease in the number of days exceeding the National Ambient Air Quality Standards (NAAQS) and a small change in total O₃ concentration. The analysis indicated that the variation of daily maximum O₃, caused by changes in emissions, explained more than 10% of the total O₃ variation in Bridgeport and East Hartford during the past 17 years. Meanwhile, a strong weekly cycle was also found in O₃ time-series data, resulting in lower O₃ concentration in urban areas than in nonur-ban areas, implying that land use and land cover have impacts on the spatial distribution of ground-level O₃ in Connecticut.     

Transport of dusts from East Asian and non-East Asian sources to Hong Kong during dust storm related events 1996–2007

Over a twelve year period from 1996 to 2007, 76 dust storm related events (as days) in Hong Kong were selected for study, based on Aluminium and Calcium concentrations in PM₁₀. Four of the 76 events reach episodic levels with exceedances of the Hong Kong air quality standards. The purpose of the study is to identify and characterize dust sources impacting Hong Kong.Global distribution of aerosols in NASA’s daily aerosol index images from TOMS and OMI, are compared to plots generated by NRL(US)’s Navy Aerosol Analysis and Prediction System. Possible source areas are assigned by computing air parcel backward trajectories to Hong Kong using the NOAA HYSPLIT model. PM₁₀ and elemental data are analyzed for crustal mass concentrations and element mass ratios.Our analysis reveals that 73 out of the 76 dust events (96%) involve non-East Asian sources-the Thar, Central/West Asian, Arabian and Sahara deserts (Saharan influence is found in 63 events), which are previously not known to affect Hong Kong. The Gobi desert is the most frequent origin of dust, affecting 68 dust events while the Taklamakan desert impacts only 30 of the dust events. The impact of the Gobi desert in March and December is apparently associated with the northeast monsoon in East Asia.Our results also show a seasonal pattern in dust impact from both East Asian and more remote sources, with a maximum in March. Dust event occurrences are conspicuously absent from summer. Dust transport to Hong Kong is commonly associated with the passage of frontal low-pressure systems.The coarse size fraction of PM₁₀ concentrations were, as indicated by Al, Ca and Fe concentrations, about 4–8 times higher during dust events. The mean Ca/Al ratios of sources involving the Taklamakan desert are notably higher than those for non-East Asian sources owing to a higher Ca content of most of the East Asian deserts. The Fe/Al ratios follow a similar trend.Contributions from the desert sources are grossly estimated where possible, by using the average Al abundance of 8% in the upper continental crust to convert the Al mass in the PM₁₀ to dust concentrations. This is done for the six events identified with air mass purely of non-East Asian origin and the two events related only to the Thar/Arabian/Sahara deserts. Results reveal that the average contribution from the non-East Asian sources (including C/W Asia) is approximately 10% and, that from the Thar/Arabian/Sahara deserts is about 8%.     

Assessment of the temporal and spatial distribution of atmospheric PCNs and their air–soil exchange using passive air samplers in Shanghai,East China

A total of 47 passive air samples and 25 soil samples were collected to study the temporal trend, distribution, and air–soil exchange of polychlorinated naphthalenes (PCNs) in Shanghai, China. Atmospheric PCNs ranged from 3.44 to 44.1 pg/m³ (average of 21.9 pg/m³) in summer and 13.6 to 153 pg/m³ (average of 40.0 pg/m³) in winter. In the soil samples, PCN concentrations were 54.7–1382 pg/g dry weight (average of 319 pg/g). Tri-CNs and tetra-CNs were two dominant homolog groups in air samples, while di-CNs were also found at comparable proportions to tri-CNs and tetra-CNs in soil samples. Most air and soil samples from the industrial and urban areas showed higher PCN concentrations than those from suburban areas. However, some soil samples in urban centers presented higher PCN concentrations than industrial areas. Analysis of PCN sources indicated that both industrial thermal process and historical usage of commercial PCN mixtures contributed to the PCN burden in most areas. The fugacity fraction results indicated a strong tendency of volatilization for lighter PCNs (tri- to hexa-CNs) in both seasons, and air–soil deposition for octa-CNs. Moreover, air–soil exchange fluxes indicate that soil was an important source of atmospheric PCNs in some areas. The results of this study provide information for use in the evaluation of the potential impact and human health risk of PCNs around the study areas.

     

Accumulation of As, Cd and selected trace elements in tubers of Scirpus maritimus L. from Doñana marshes (South Spain)

The collapse of a pyrite-mining, tailing dam on 1998 contaminated an area of 4286 ha along the Agrio and Guadiamar river valleys in southern Spain. Over 2700 ha of the Do?ana marshes, an important wintering area for wetland European birds, were contaminated. This study reports analyses of the tubers of Scirpus maritimus (an important food for greylag geese, Anser anser) collected in 2000 in the "Entremuros" (spill-affected area) and in nearby unaffected Do?ana marshes (control areas). In the spill-affected area mean tuber tissue concentrations of Cd (0.25 mg kg-1) and Zn (61 mg kg-1) were greater than in those tubers from the control area (0.02 mg kg-1 for Cd, and 22 mg kg-1 for Zn); values of Cd and Zn in "Entremuros" (samples collected two years after the mine spill) were much smaller than those reported only a few months after the accident. Trace elements (As, Fe, Mn and Tl, and to a lesser extent Cd and Pb) showed a preferential accumulation in the outer skin of tubers. Surprisingly, concentrations of As and Fe were greater in tubers from some marsh sites not affected by the mine-spill than in tubers from the "Entremuros". We suggest that relic river channels within the Do?ana marshes may be contaminated by trace elements from historic mining activities. An exhaustive study of macrophytes and other plant species in this area is recommended to identify potential risks to wildlife.     

A review of plant–pharmaceutical interactions: from uptake and effects in crop plants to phytoremediation in constructed wetlands

Pharmaceuticals are commonly found both in the aquatic and the agricultural environments as a consequence of the human activities and associated discharge of wastewater effluents to the environment. The utilization of treated effluent for crop irrigation, along with land application of manure and biosolids, accelerates the introduction of these compounds into arable lands and crops. Despite the low concentrations of pharmaceuticals usually found, the continuous introduction into the environment from different pathways makes them ‘pseudo-persistent’. Several reviews have been published regarding the potential impact of veterinary and human pharmaceuticals on arable land. However, plant uptake as well as phytotoxicity data are scarcely studied. Simultaneously, phytoremediation as a tool for pharmaceutical removal from soils, sediments and water is starting to be researched, with promising results. This review gives an in-depth overview of the phytotoxicity of pharmaceuticals, their uptake and their removal by plants. The aim of the current work was to map the present knowledge concerning pharmaceutical interactions with plants in terms of uptake and the use of plant-based systems for phytoremediation purposes.     

Distribution of Hg,As and Se in material and flue gas streams from preheater–precalciner cement kilns and vertical shaft cement kilns in China

The aim of this study was to evaluate the behavior of Hg, As, and Se in cement production. Two types of cement plants were studied, including the vertical shaft kiln (VSK) and preheater–precalciner kiln (PPK) processes. Determination of Hg, As, and Se in the main material and gas streams were performed. It was found that recycling of particulate matter captured by an air pollution control device caused a significant enrichment of Hg and As inside both processes. The total quantity of Hg entering the process and the quantity emitted to the atmosphere were found to be 10–109 and 6.3–38 mg, respectively, per ton of clinker produced. The average Hg emission was calculated to be around 41% of the total mercury input. The emissions found complied with the European Union (EU) limit and exceeded partly the U.S. limit. Furthermore, it was found that oxidized mercury was the dominant species in the PPK process, whereas the reduced form was dominant in the VSK process, due to the oxidizing and reducing gas conditions, respectively. Regarding the distribution of As and Se, the major amounts were bound to the solid materials, that is, cement clinker and particulate matter. Based on cement production data in China in 2013, the annual emissions of Hg and As were estimated to be in the range of 8.6–52 and 4.1–9.5 tons, respectively.

Implications: There are fairly limited studies on Hg, As, and Se measurements from cement manufacturing facilities in China, and even more limited studies on the behavior in vertical shaft kilns. The needs for increased emission reduction efforts in energy-intensive industries are globally recognized, and an improved understanding of the processes ongoing in a cement kilns system is decisive. Since the processes are complex and almost impossible to recreate in the laboratory, field measurements are indeed important. The findings in the present study were solely based on field measurements and the data are considered to be valuable for the further development of emission reduction technology.