Sources,distribution, and acidity of sulfate–ammonium aerosol in the Arctic in winter–spring

We use GEOS-Chem chemical transport model simulations of sulfate–ammonium aerosol data from the NASA ARCTAS and NOAA ARCPAC aircraft campaigns in the North American Arctic in April 2008, together with longer-term data from surface sites, to better understand aerosol sources in the Arctic in winter–spring and the implications for aerosol acidity. Arctic pollution is dominated by transport from mid-latitudes, and we test the relevant ammonia and sulfur dioxide emission inventories in the model by comparison with wet deposition flux data over the source continents. We find that a complicated mix of natural and anthropogenic sources with different vertical signatures is responsible for sulfate concentrations in the Arctic. East Asian pollution influence is weak in winter but becomes important in spring through transport in the free troposphere. European influence is important at all altitudes but never dominant. West Asia (non-Arctic Russia and Kazakhstan) is the largest contributor to Arctic sulfate in surface air in winter, reflecting a southward extension of the Arctic front over that region. Ammonium in Arctic spring mostly originates from anthropogenic sources in East Asia and Europe, with added contribution from boreal fires, resulting in a more neutralized aerosol in the free troposphere than at the surface. The ARCTAS and ARCPAC data indicate a median aerosol neutralization fraction [NH₄⁺]/(2[SO₄^2?] + [NO₃^?]) of 0.5 mol mol^?1 below 2 km and 0.7 mol mol^?1 above. We find that East Asian and European aerosol transported to the Arctic is mostly neutralized, whereas West Asian and North American aerosol is highly acidic. Growth of sulfur emissions in West Asia may be responsible for the observed increase in aerosol acidity at Barrow over the past decade. As global sulfur emissions decline over the next decades, increasing aerosol neutralization in the Arctic is expected, potentially accelerating Arctic warming through indirect radiative forcing and feedbacks.     

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.     

Determination of cyclic volatile methylsiloxanes in water,sediment, soil,biota, and biosolid using large-volume injection–gas chromatography–mass spectrometry

Several methods were developed to detect the cyclic volatile methylsiloxanes (cVMSs) including octamethylcyclotetrasiloxane (D4), decamethylcyclopentasiloxane (D5), and dodecamethylcyclohexasiloxane (D6) in water, sediment, soil, biota, and biosolid samples. Analytical techniques employed to optimize measurement of this compound class in various matrices included membrane-assisted solvent extraction in water, liquid–solid extraction for sediment, soil, biota, and biosolid samples. A subsequent analysis of the extract was conducted by large-volume injection–gas chromatography−mass spectrometry (LVI−GC−MS). These methods employed no evaporative techniques to avoid potential losses and contamination of the volatile siloxanes. To compensate for the inability to improve detection limits by concentrating final sample extract volumes we used a LVI–GC–MS. Contamination during analysis was minimized by using a septumless GC configuration to avoid cVMS’s associated with septum bleed. These methods performed well achieving good linearity, low limits of detection, good precision, recovery, and a wide dynamic range. In addition, stability of cVMS in water and sediment was assessed under various storage conditions. D4 and D5 in Type-I (Milli-Q) water stored at 4 °C were stable within 29 d; however, significant depletion of D6 (60–70%) occurred only after 3 d. Whereas cVMS in sewage influent and effluent were stable at 4 °C within 21 d. cVMS in sediment sealed in amber glass jars at −20 °C and in pentane extracts in vials at −15 °C were stable during 1 month under both storage conditions.     

Atmospheric concentrations,gaseous–particulate distribution,and carcinogenic potential of polycyclic aromatic hydrocarbons in Assiut,Egypt

The concentrations of 15 priority PAHs were determined in the atmospheric gaseous and particulate phases from nine sites across Assiut City, Egypt. While naphthalene, acenaphthene, and fluorene were the most abundant in the gaseous phase with average concentrations of 377, 184, and 181 ng/m³, benzo[b]fluoranthene, chrysene, and benzo[g,h,i]perylene showed the highest levels in the particulate phase with average concentrations of 76, 6, and 52 ng/m³. The average total atmospheric concentration of target PAHs (1,590 ng/m³) indicates that Assiut is one of the highest PAH-contaminated areas in the world. Statistical analysis revealed a significant difference between the levels of PAHs in the atmosphere of urban and suburban sites (P?=?0.029 and 0.043 for gaseous and particulate phases, respectively). Investigation of diagnostic PAH concentration ratios revealed vehicular combustion and traffic exhaust emissions as the major sources of PAHs with a higher contribution of gasoline rather than diesel vehicles in the sampled areas. Benzo[a]pyrene has the highest contribution (average?=?32, 4 % for gaseous and particulate phases) to the total carcinogenic activity (TCA) of atmospheric PAHs. While particulate phase PAHs have higher contribution to the TCA, gaseous phase PAHs present at higher concentrations in the atmosphere are more capable of undergoing atmospheric reactions to form more toxic derivatives.     

Fifteen years of monitoring of POPs in the breast milk, Czech Republic, 1994–2009: trends and factors

Background, aim and scope

The breast milk has been recommended to carry out as a monitoring tool for effectiveness evaluation of the Stockholm Convention on Persistent Organic Pollutants (POPs). Polychlorinated biphenyls (PCBs), dichlorodiphenyltrichloro-ethane (DDT) and its metabolites (DDX), hexachlorbenzene (HCB) and isomers of hexachlocyklohexane (HCHs) have been monitored in the breast milk of nursing mothers in the Czech Republic since 1994 as a part of The Environmental Health Monitoring System. Knowledge about long-term POPs distribution and accumulation in the human body is crucial to understanding uptake, degradation and subsequent effects as well as to conduct risk assessments. The main aim of this study is to evaluate 15-years long-term trends of selected POPs in human milk in the Czech Republic and to elucidate the questionnaire information about the age, parity and social habits, to the final concentrations. This effectiveness evaluation of POPs restriction is quite precisely after 15-years monitoring campaigns.

Materials, methods and results

The human milk samples (4,753 samples) were analysed for a number of chlorinated organic chemicals including PCBs and selected chlorinated pesticides (OCPs, HCB, HCHs, DDX). The relative change of concentration per year for all chemicals was analysed. The remaining percentages of POPs in breast milk in comparison to 1994 are also expressed. Czech population half-lives of POPs in breast milk, derived from either linear or exponential models were computed.

Conclusions and perspectives

The long-term data indicates a continuation of a decreasing trend of POPs concentrations on breast milk. Our study did not confirm lactation and parity as an important outflux resulting in the decrease in concentrations in mothers, which is in the antagonism with most of the studies. The higher BMI was associated with higher amounts of HCB and lower amounts of higher chlorinated PCBs. The results confirm the effectiveness of restrictions of POPs usage in the Czech Republic. This ongoing long-term study is very useful tool for parametric effectiveness evaluation of Stockholm Convention.     

Multiscale analysis of factors affecting food security in China, 1980–2017

Environmental Science and Pollution Research - Food security is an important issue affecting people’s lives and social stability. Clarifying levels of food security and the factors affecting...     

Implications of Rural–Urban Migration for Conservation of the Atlantic Forest and Urban Growth in Misiones,Argentina (1970–2030)

Global trends of increasing rural–urban migration and population urbanization could provide opportunities for nature conservation, particularly in regions where deforestation is driven by subsistence agriculture. We analyzed the role of rural population as a driver of deforestation and its contribution to urban population growth from 1970 to the present in the Atlantic Forest of Argentina, a global conservation priority. We created future land-use-cover scenarios based on human demographic parameters and the relationship between rural population and land-cover change between 1970 and 2006. In 2006, native forest covered 50% of the province, but by 2030 all scenarios predicted a decrease that ranged from 18 to 39% forest cover. Between 1970 and 2001, rural migrants represented 20% of urban population growth and are expected to represent less than 10% by 2030. This modeling approach shows how rural–urban migration and land-use planning can favor nature conservation with little impact on urban areas.     

A Survey of Ambient Air Levels of Lead in El Paso,Texas from 1972–1979

In an era when the cost of compliance with state and federal environmental laws is rapidly rising, sometimes entities, such as operators of waste sites, are unable to pay these and other operating costs and are forced to file for bankruptcy. Citing Midlantic Nat'l Bank v. N.J. Dep't of Envtl. Protection and state environmental laws, bankruptcy trustees may be suing PRPs in bankruptcy courts to share the costs to clean up debtors' waste sites. This article suggests strategies by which PRPs can avoid litigating such lawsuits in the bankruptcy courts and instead resolve them before state and/or federal forums—where they properly belong.     

Seasonal variability of radon-derived fetch regions for Sado Island,Japan, based on 3 years of observations: 2002–2004

Three years of hourly atmospheric radon measurements at Sado Island (Japan) are discussed and compared with corresponding measurements at Gosan (South Korea), and Hok Tsui (China). In conjunction with back trajectory analysis, Sado radon data are used to characterise the seasonal variability in fetch regions of air masses subject to extremes of terrestrial influence. In winter, fetch regions of air masses that have experienced the greatest terrestrial influence covered southern Siberia; in summer, the terrestrial fetch was dominated by Japan; throughout the remaining months the terrestrial fetch encompassed the Korean Peninsula and far eastern China. Summer radon data are then used to estimate the radon flux from central Honshu (23.5 mBq m^?2 s^?1), which varied regionally between 10.6 and 47.9 mBq m^?2 s^?1. The Sado radon record reported here completes a 4-site, multi-year dataset of hourly radon concentrations across East Asia and the central Pacific (spanning 16° of latitude), which constitutes a unique evaluation tool for transport and mixing schemes of atmospheric and chemical transport models.     

Temporal and spatial trends of PCBs,DDTs, HCHs,and HCB in Swedish marine biota 1969–2012

In the 1960s, the Baltic Sea was severely polluted by organic contaminants such as PCBs, HCHs, HCB, and DDTs. Elevated concentrations caused severe adverse effects in Baltic biota. Since then, these substances have been monitored temporally and spatially in Baltic biota, primarily in herring (Clupea harengus) and in guillemot (Uria aalge) egg, but also in cod (Gadus morhua), perch (Perca fluviatilis), eelpout (Zoarces viviparous), and blue mussel (Mytilus edulis). These chemicals were banned in Sweden in the late 1970s/early 1980s. Since the start of monitoring, overall significant decreases of about 70–90 % have been observed. However, concentrations are still higher in the Baltic Sea than in, for example, the North Sea. CB-118 and DDE exceed the suggested target concentrations (24 µg kg^?1 lipid weight and 5 µg kg^?1 wet weight, respectively) at certain sites in some of the monitored species, showing that concentrations may still be too high to protect the most sensitive organisms.     

Multivariate Space Analysis of the Major Precipitation Ions over Europe, 1986–1997

ABSTRACT

The annual average concentrations (1986–1997) of the major ions SO₄ ^2-, NO₃ ^-, Cl^-, NH₄+, Na+, Mg²+, Ca²+, and K+ in precipitation are analyzed for selected EMEP stations. The objective is to determine the ion patterns or typologies in precipitation by principal component analysis (PCA) combined with a cluster analysis. SO₄ ^2- and NO₃ ^- ions are predominant in central and eastern Europe. This area corresponds to high emissions of SO₂ and NO₂. Sea spray ions are predominant in coastal sites. The soil components show an important contribution in southern Europe, possibly due to the soil dust transported from northern Africa.     

Emission inventory for greenhouse gases in the City of Barcelona, 1987–1996

Emissions of greenhouse gases for the City of Barcelona are estimated for the period 1987–1994. The sources considered are: public and private transportation; industrial, commercial and domestic activities; and municipal solid waste disposal. The results show that the main source of CO₂ emissions in Barcelona is private vehicle transportation, which accounts, as an average for the period studied, for 35% of total emissions. The second most important source is the municipal solid waste landfill facility of the city (24% of total emissions). The percentages for the remaining sources under consideration were: 14% electricity, 12% natural gas, 5% incineration, and 3% liquefied petroleum gases. However, the values for CO₂ emissions per inhabitant over the period studied are lower than those for any other industrialized city available for comparison. This is closely related to the high percentage of electricity generation from nuclear power stations and hydro power facilities, and also to the extensive use of natural gas for domestic uses.     

Microscopy and chemistry of particles collected on TEOM filters: Swansea,south Wales, 1998–1999

Tapered element oscillating microbalances (TEOMs) are used in the UK Automatic Monitoring Network for the continuous measurement of ambient airborne particles. Used TEOM filters from Swansea, Cardiff and Pembroke were examined under high-resolution field emission scanning electron microscopy (FESEM). Clusters of calcium sulphate crystals, gypsum (CaSO₄·2H₂O) and anhydrite (CaSO₄) were abundant on spring and summer filters, and not present on autumn and winter filters. From textural considerations, the sulphates must have crystallised on the filter surfaces, either by dissolution and recrystallisation of CaSO₄ collected as particles, or by direct precipitation from saline water collected on the filters; in much the same way as the formation of ‘desert roses’ by the evaporation of saline pore waters in desert sands. The proposed mechanism for the formation of these crystals has two important implications. Firstly, if the filters are episodically saturated with water, then on occasion the recorded masses will consist of both particles plus water, causing errors in the results of continuous monitoring; an important consideration for epidemiological studies based on TEOM data. Secondly, past toxicological experiments undertaken on TEOM-derived ‘PM10’ may have investigated material containing a significant component of in situ formed crystals, rather than the original PM10.     

Characteristics of precipitation chemistry at Lushan Mountain, East China: 1992–2009

Introduction

Trends in precipitation pH and conductivity during 1992?C2009, and in ionic compositions from January 2007 to June 2009, are reported from Lushan Mountain, one of the highest mountains in mid-east China. Annual mean pH was in the range of 4.35?C5.01 and showed a statistically very significant (P?P?Results and discussions Over the period of study, Lushan Mountain received more rainfall in spring and summer. The pH values varied seasonally with winter minima. The winter multiyear seasonal mean pH was 4.35. The corresponding summer value was 4.88. SO ₄ ^2? and NO ₃ ^? were the main anions, and NH ₄ ⁺ and Ca²⁺ the main cations. The anion to cation ratio was 0.8?C1.0, and that of [SO ₄ ^2? ] to [NO ₃ ^? ] was 2.4-3.0, much lower than that of the 1980s. However, sulfuric acid was still the main acid present. The ratio of [NH ₄ ⁺ ] to [Ca²⁺] was about 1.0, suggesting that these two alkaline substances provided close acid neutralizing capacity. The ratio of [Cl^?] to [Na⁺] was about 0.67, somewhat lower than that of natural precipitation.

Conclusions

Ionic composition varied seasonally and was closely correlated to the amounts of rainfall and pollution. Trajectory analyses showed that the trajectories to Lushan Mountain could be classified in six clusters and trajectories originating from the South Sea and the areas surrounding Lushan Mountain had the greatest impacts on precipitation chemistry.     

Seasonal variations of particle-associated nitrosamines by gas chromatography–mass spectrometry in the atmospheric environment of Zonguldak, Turkey

A gas chromatography–mass spectrometry method has been proposed for the determination of low-level mutagenic and carcinogenic nitrosamines in particulate matter. The method includes the collection of particulate matters (PM_2.5 and PM₁₀) using a dichotomous Partisol 2025 sampler and extraction of the compounds from aqueous solution with dichloromethane/2-propanol after sonication with a slightly basic water solution prior to their GC-MS analysis in electron impact mode. The obtained recoveries of nitrosamines ranged from 92.4 to 99.2 %, and the precision of this method, as indicated by the relative standard deviations, was within the range of 0.95–2.46?%. The detection limits obtained from calculations using the GC-MS results based on S/N?=?3 were found within the range from 4 to 22 pg/m³. The predominant nitrosamines determined in particulate matter were N-nitrosodimethylamine, N-nitrosodiethylamine, N-nitrosodibutylamine and N-nitrosomorpholine. Furthermore, N-mono- and dinitrosopiperazine and N-nitrosoethylbutylamine were also determined. N-dinitrosopiperazine was detected in PM_2.5 samples at the highest concentrations of up to 22.85 ng/m³ and in PM_2.5–10 samples at concentrations up to 7.60 ng/m³ in winter, whereas it was found in PM_2.5 samples up to 5.15 ng/m³ and in PM_2.5–10 samples up to 3.12 ng/m³ in summer. The total concentrations of nitrosamines were up to 161.4 ng/m³ in fine and 53.90 ng/m³ in coarse fractions in winter, whereas in summer were up to 35.24 and 12.60 ng/m³, respectively. The concentration levels of nitrosamines fluctuated significantly within a year, with higher means and peak concentrations in the winter compared to that in the summertime. The seasonal variations of particle-associated nitrosamine concentrations were investigated together with their relationships with meteorological parameters using Pearson’s correlation analysis in the winter and summer periods. Analysis of variance was used to determine which concentrations of nitrosamines were statistically different from one another and, together with meteorological parameters and discriminant analysis, was used to classify the particle samples by particle size according to seasons. The classification results of the particle samples in different seasons were very satisfactory, allowing 99.5 % of cases to be correctly grouped.     

Water–gas exchange of organochlorine pesticides at Lake Chaohu, a large Chinese lake

Organochlorine pesticides (OCPs), a potential threat to ecosystems and human health, are still widely residual in the environment. The residual levels of OCPs in the water and gas phase were monitored in Lake Chaohu, a large Chinese lake, from March 2010 to February 2011. Nineteen types of OCPs were detected in the water with a total concentration of 7.27?±?3.32 ng/l. Aldrin, DDTs and HCHs were the major OCPs in the water, accounting for 38.3 %, 28.9 % and 23.6 % of the total, respectively. The highest mean concentration (12.32 ng/l) in the water was found in September, while the lowest (1.74 ng/l) was found in November. Twenty types of gaseous OCPs were detected in the atmosphere with a total concentration of 542.0?±?636.5 pg/m³. Endosulfan, DDTs and chlordane were the major gaseous OCPs in the atmosphere, accounting for 48.9 %, 22.5 % and 14.4 % of the total, respectively. The mean concentration of gaseous OCPs was significantly higher in summer than in winter. o,p′-DDE was the main metabolite of DDT in both the water and gas phase. Of the HCHs, 52.3 % existed as β-HCH in the water, while α-HCH (37.9 %) and γ-HCH (30.9 %) were dominant isomers in the gas phase. The average fluxes were ?21.11, ?3.30, ?152.41, ?35.50 and ?1314.15 ng/(m²?day) for α-HCH, γ-HCH, HCB, DDT and DDE, respectively. The water–gas exchanges of the five types of OCPs indicate that water was the main potential source of gaseous OCPs in the atmosphere. A sensitivity analysis indicated that the water-gas flux of α-HCH, γ-HCH and DDT is more vulnerable than that of HCB and DDE to the variation of the parameters. The possible source of the HCHs in the water was from the historical usage of lindane; however, that in the air was mainly from the recent usage of lindane. The technical DDT and dicofol might be the source of DDTs in the water and air.     

Characteristics of ambient C2–C11 non-methane hydrocarbons in metropolitan Nagoya,Japan

To understand the characteristics of non-methane hydrocarbon (NMHC) abundance in an urban air of Nagoya, one of the metropolitan areas of Japan, 48 species of C₂–C₁₁ NMHCs were measured with a measurement system, developed in this study, by using gas chromatography with flame ionization detection (GC/FID) continuously for one year from December 2003 to November 2004.Annual mean concentration of NMHCs in normal and propylene equivalent (PE) in Nagoya was compared with those in four urban areas of Seoul, London, Lille, and Dallas to extract characteristics of urban air. While the absolute values of the normal and PE concentrations of alkanes, alkenes, alkyne, and aromatics were significantly different among these urban areas, the proportions of each chemical group to the total NMHC were not so different.In Nagoya, the total normal concentration was high from November to February and low from June to August. The pattern of the seasonal variation was influenced mainly by that of alkanes. On the other hand, the total PE concentration was high from July to December and low from January to June. The pattern of the seasonal variation was influenced mainly by those of alkenes and aromatics. Particularly the normal concentration of isoprene was high from May to September because of large emission associated with activity of plants. As the results, in summer, the PE concentration of isoprene was especially high, and its contribution to the total NMHCs measured in this study was approximately 40%. The total PE concentrations were high in summer when the concentration of OH radicals is also high, suggesting that the productions of ozone and secondary organic aerosol (SOA) are likely to be promoted in summer of Nagoya.     

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.