Atmospheric nitrogen fluxes at the Belgian coast: 2004–2006

Daily and seasonal variations in dry and wet atmospheric nitrogen fluxes have been studied during four campaigns between 2004 and 2006 at a coastal site of the Southern North Sea at De Haan (Belgium) located at coordinates of 51.1723° N and 3.0369° E. Concentrations of inorganic N-compounds were determined in the gaseous phase, size-segregated aerosol (coarse, medium, and fine), and rainwater samples. Dissolved organic nitrogen (DON) was quantified in rainwater. The daily variations in N-fluxes of compounds were evaluated with air-mass backward trajectories, classified into the main air-masses arriving at the sampling site (i.e., continental, North Sea, and Atlantic/UK/Channel).The three, non-episodic campaigns showed broadly consistent fluxes, but during the late summer campaign exceptionally high episodic N-deposition was observed. The average dry and wet fluxes for non-episodic campaigns amounted to 2.6 and 4.0 mg N m^?2 d^?1, respectively, whereas during the episodic late summer period these fluxes were as high as 5.2 and 6.2 mg N m^?2 d^?1, respectively.Non-episodic seasons/campaigns experienced average aerosol fluxes of 0.9–1.4 mg N m^?2 d^?1. Generally, the contribution of aerosol NH₄⁺ was more significant in the medium and fine particulate fractions than that of aerosol NO₃^?, whereas the latter contributed more in the coarse fraction, especially in continental air-masses. During the dry mid-summer campaign, the DON contributed considerably (～15%) to the total N-budget.Exceptionally high episodic aerosol-N inputs have been observed for the late summer campaign, with especially high deposition rates of 3.6 and 2.9 mg N m^?2 d^?1 for Atlantic/UK/Channel and North Sea-continental (mixed) air-masses, respectively. During this pollution episode, the flux of NH₄⁺ was dominating in each aerosol fraction/air-mass, except for coarse continental aerosols. High deposition of gaseous-N was also observed in this campaign with an average total N-flux of 2–2.5-times higher than in other campaigns.     

Increased nitrogen in runoff and soil following 13 years of experimentally increased nitrogen deposition to a coniferous-forested catchment at Gårdsjön, Sweden

Beginning in 1991, we have added nitrogen (N) to the 0.5-ha, N-poor, coniferous-forested catchment G2 NITREX at G?rdsj?n, Sweden, to investigate the consequences of chronic elevated N deposition. We have added 40 kg N ha-1 yr-1 in fortnightly doses of NH4NO3 to the ambient 15 kg N ha-1 yr-1 by means of a sprinkling system. NO3 concentrations in runoff increased during 13 years from<1 to 70 microeq L-1, and in 2004 comprised about 10% of N input. Inhibition of NO3 immobilisation due to increased availability of NH4 might explain the increased leaching of NO3. C and N pools in the forest floor increased but C/N ratio has not changed. The increase in NO3 leaching thus occurred independently of change in C/N ratio. The results from G?rdsj?n demonstrate that increased leaching of inorganic N and decrease in C/N ratio respond to increased N deposition at greatly different time scales.     

Interaction of nitrogen dioxide (NO2) with a monolayer of oleic acid at the air–water interface – A simple proxy for atmospheric aerosol

The reactions between atmospheric oxidants and organic amphiphiles at the air–water interface of an aerosol droplet may affect the size and critical supersaturation required for cloud droplet formation. We demonstrate that no reaction occurs between gaseous nitrogen dioxide (1000 ppm in air) and a monolayer of an insoluble amphiphile, oleic acid (cis-9-octadecenoic acid), at the air–water interface which removes material from the air–water interface. We present evidence that the NO₂ isomerises the cis-9-octadecenoic (oleic) acid to trans-9-octadecenoic (elaidic) acid. The study presented here is important for future and previous studies of (1) the reaction between the nitrate radical, NO₃, and thin organic films as NO₂ is usually present in high concentrations in these experimental systems and (2) the effect of NO₂ air pollution on the unsaturated fatty acids and lipids found at the air–liquid surface of human lung lining fluid.     

Can the foliar nitrogen concentration of upland vegetation be used for predicting atmospheric nitrogen deposition? Evidence from field surveys

The deposition of atmospheric nitrogen can be enhanced at high altitude sites as a consequence of cloud droplet deposition and orographic enhancement of wet deposition on hills. The degree to which the increased deposition of nitrogen influences foliar nitrogen concentration in a range of upland plant species was studied in a series of field surveys in northern Britain. A range of upland plant species sampled along altitudinal transects at sites of known atmospheric nitrogen deposition showed marked increases in foliar nitrogen concentration with increasing nitrogen deposition and altitude (and hence with decreasing temperature). For Nardus stricta L., Deschampsia flexuosa (L.) Trin., Calluna vulgaris (L.) Hull, Erica cinerea L. and Hylocomium splendens (Hedw.) Br. Eur. on an unpolluted hill, foliar nitrogen increased by 0.07, 0.12, 0.15, 0.08 and 0.04% dry weight respectively for each 1 kg ha(-1) year(-1) increase in nitrogen deposition. Most species showed an approximately linear relationship between foliar nitrogen concentration and altitude but no trend with altitude for foliar phosphorus concentration. This provided evidence that the tissue nutrient status of upland plants reflects nutrient availability rather than the direct effects of climate on growth. However, differences in the relationship between foliar nitrogen concentration and atmospheric nitrogen deposition for N. stricta sampled on hills in contrasting pollution climates show that the possibility of temperature-mediated growth effects on foliar nitrogen concentration should not be ignored. Thus, there is potential to use upland plant species as biomonitors of nitrogen deposition, but the response of different species to nitrogen addition, in combination with climatic effects on growth, must be well characterised.     

Field evaluations of newly available “interference-free” monitors for nitrogen dioxide and ozone at near-road and conventional National Ambient Air Quality Standards compliance sites

Long-standing measurement techniques for determining ground-level ozone (O₃) and nitrogen dioxide (NO₂) are known to be biased by interfering compounds that result in overestimates of high O₃ and NO₂ ambient concentrations under conducive conditions. An increasing near-ground O₃ gradient (NGOG) with increasing height above ground level is also known to exist. Both the interference bias and NGOG were investigated by comparing data from a conventional Federal Equivalent Method (FEM) O₃ photometer and an identical monitor upgraded with an “interference-free” nitric oxide O₃ scrubber that alternatively sampled at 2 m and 6.2 m inlet heights above ground level (AGL). Intercomparison was also made between a conventional nitrogen oxide (NO_x) chemiluminescence Federal Reference Method (FRM) monitor and a new “direct-measure” NO₂ NO_x 405 nm photometer at a near-road air quality measurement site. Results indicate that the O₃ monitor with the upgraded scrubber recorded lower regulatory-oriented concentrations than the deployed conventional metal oxide–scrubbed monitor and that O₃ concentrations 6.2 m AGL were higher than concentrations 2.0 m AGL, the nominal nose height of outdoor populations. Also, a new direct-measure NO₂ photometer recorded generally lower NO₂ regulatory-oriented concentrations than the conventional FRM chemiluminescence monitor, reporting lower daily maximum hourly average concentrations than the conventional monitor about 3 of every 5 days.

Implications: Employing bias-prone instruments for measurement of ambient ozone or nitrogen dioxide from inlets at inappropriate heights above ground level may result in collection of positively biased data. This paper discusses tests of new regulatory instruments, recent developments in bias-free ozone and nitrogen dioxide measurement technology, and the presence/extent of a near-ground O₃ gradient (NGOG). Collection of unbiased monitor inlet height–appropriate data is crucial for determining accurate design values and meeting National Ambient Air Quality Standards.     

Use of Calluna vulgaris to detect signals of nitrogen deposition across an urban–rural gradient

Densely populated cities can experience high concentrations of traffic-derived pollutants, with oxides of nitrogen and ammonia contributing significantly to the overall nitrogen (N) budget of urban ecosystems. This study investigated changes in the biochemistry of in situ Calluna vulgaris plants to detect signals of N deposition across an urban–rural gradient from central London to rural Surrey, UK. Foliar N concentrations and δ¹⁵N signatures were higher, and C/N ratios lower, in urban areas receiving the highest rates of N deposition. Plant phosphorus (P) concentrations were also highest in these areas, suggesting that elevated rates of N deposition are unlikely to result in progressive P-limitation in urban habitats. Free amino acid concentrations were positively related to N deposition for asparagine, glutamine, glycine, phenylalanine, isoleucine, leucine and lysine. Overall, relationships between tissue chemistry and N deposition were similar for oxidised, reduced and total N, although the strength of relationships varied with the different biochemical indicators. The results of this study indicate that current rates of N deposition are having substantial effects on plant biochemistry in urban areas, with likely implications for the biodiversity and functioning of urban ecosystems.     

Sources and concentrations of gaseous and particulate reduced nitrogen in the city of Münster (Germany)

Atmospheric ammonia mixing ratios and the main inorganic ions NH₄⁺, NO₃⁻ and SO₄²⁻ of size-resolved particles in the range from 0.05 to 10 μm were measured at an urban site in Münster, Germany. High mixing ratios of ammonia with a median of 5.2 ppb and a maximum of 50 ppb were detected. The mass fraction of submicron particles was much higher during the day than at night. At night, a greater particle mass and an increased presence of particulate nitrate was measured. Recurring patterns of particle distribution were distinguished and their characteristics analysed. In half of the measurements, the accumulation mode was clearly dominating, which is an indication of aged aerosol. In some measurements, higher concentrations of fine particles were found indicating particle formation. In these cases, a smaller particle mass and about four times greater ratios of ammonia versus ammonium concentrations were observed. These data show that ammonia contributes considerably to the formation of secondary particulate material.     

Ambient sulfur dioxide,nitrogen dioxide,and ammonia at ten background and rural sites in China during 2007–2008

We present two years (January 2007–December 2008) of atmospheric SO₂, NO₂ and NH₃ measurements from ten background or rural sites in nine provinces in China. The measurements were made on a monthly basis using passive samplers under careful quality control. The results show large geographical and seasonal variations in the concentrations of these gases. The mean SO₂ concentration varied from 0.7 ± 0.4 ppb at Waliguan on Qinghai Plateau to 67.3 ± 31.1 ppb at Kaili in Guizhou province. The mean NO₂ concentration ranged from 0.6 ± 0.4 ppb at Waliguan to 23.9 ± 6.9 ppb at Houma in southern Shanxi. The mean NH₃ concentration ranged from 2.8 ± 3.0 ppb at Shangdianzi in northeastern Beijing to 13.7 ± 8.4 ppb at Houma. At most sites, SO₂ and NO₂ peaked in winter and reached minima in summer, while NH₃ showed maximum values in summer and lower values in cold seasons. On the whole, the geographical distributions of the observed gas concentrations are consistent with those of emissions. The ground measurements of SO₂ and NO₂ are contrasted to the SCIAMACHY SO₂ and OMI NO₂ tropospheric columns, respectively. Although the satellite data can capture the main features of emissions and concentrations of SO₂, they do not reflect the variations of SO₂ in the surface layer. The situation is better for the case of NO₂. The OMI NO₂ columns capture the geographical differences in the ground NO₂ and correlate fairly well with the ground levels of NO₂ at six of the ten sites.     

Variability-lifetime relationship of VOCs observed at the Sonnblick Observatory 1999—estimation of HO-densities

An extensive dataset of VOC measurements was collected at the Sonnblick Observatory, Austria (3106 m) in Fall/Winter 1999/2000, showing high mixing ratios of anthropogenic and biogenic VOCs at this high altitude site due to upward mixing of air masses (Geophys. Res. Lett. 2F (2001) 507). Here we give an interpretation of proton-transfer-reaction (PTR-MS) mass scans obtained in November 1999 based on fragmentation data, GC-PTR-MS analysis and the variability-lifetime relationship, described by the power law, σ(ln(x))=Aτ^−b. The variability-lifetime plot of anthropogenic VOCs gave a proportionality factor A of 1.40 and a,b exponent (sink term) of 0.44 and allowed an estimate of average HO-densities on the order of (1.5±0.4)×10⁵ molecules cm⁻³. Additionally we were able to indirectly determine a diurnal HO-profile with peak values of (1.3±0.5)×10⁶ molecules cm⁻³ around midday. HO-reaction rate coefficients for higher aldehydes (heptanal to nonanal) were estimated due to photochemical losses during a stagnant air episode (27 November) and from the variability-lifetime relationship. Combining long term PTR-MS analysis of VOCs and the variability-lifetime method provides a valuable tool for assessing the dominant cause of the variability in VOC concentrations. This information is essential in understanding the sources and photochemical processing of VOCs detected in ambient air at field measurement sites.     

Chemistry of fog waters in California's Central Valley—Part 3: concentrations and speciation of organic and inorganic nitrogen

Although organic nitrogen (ON) has been found to be a ubiquitous and significant component in wet and dry deposition, almost nothing is known about its concentration or composition in fog waters. To address this gap, we have investigated the concentration and composition of ON in fog waters collected in Davis, in California's Central Valley. Significant quantities of dissolved organic nitrogen (DON) were found in these samples, with a median concentration of 303 μM N (range=120–1630 μM N). DON typically represented approximately 16% of the total dissolved nitrogen (inorganic+organic) in Davis fog waters. The median concentration of nitrogen in free amino acids and alkyl amines was 16 μM N (range=3.8–120 μM N), which accounted for 3.4% of the DON in Davis fogs. Thus, although the absolute concentrations of free amino compounds were significant, they were only a minor component of the DON pool. Combined amino nitrogen (e.g., proteins and peptides) was present at higher concentrations and accounted for 6.1–29% (median=16%) of DON. Overall, free and combined amino compounds typically accounted for a median value of 22% of DON in the fog waters.The high concentrations of DON found, and the fact that amino and other N-containing organic compounds can serve as nitrogen sources for microorganisms and plants, indicate that atmospheric ON compounds likely play an important role in nitrogen cycling in the Central Valley. In addition, due to the basicity of some N functional groups, ON compounds likely contribute to the previously observed acid buffering capacity of Central Valley fog waters. Finally, a comparison of fog waters with fine particles (PM_2.5) collected from the same site during the same period of time indicated that the median concentrations (mol N m⁻³-air) of total water-soluble ON, free amino nitrogen and total amino nitrogen were very similar in the fog water and PM_2.5. Given the high water solubility of many organic N compounds, this result suggests that ON might contribute to the hygroscopic properties of atmospheric particles.     

Determination of the applicability of CERCLA's petroleum exclusion at contaminated sites – focus on metals

Areas impacted by petroleum refining and handling operations may become subject to CERCLA enforcement. Because of CERCLA's petroleum exclusion clause, determining whether contamination in a CERCLA Site originated from petroleum products or hazardous wastes becomes important. Because certain metals are typically enriched in wastes relative to petroleum products and background soils, knowledge of metal contents in these potential end member metal sources is an important step towards contaminant source identification in soils and sediments. In LNAPL plumes, metal content, particularly lead, may be claimed to be the result of wastes mishandling and not due only to the presence of leaded gasoline in the plume. Analysis of the percent gasoline in the plume and accounting for weathering are steps to determining whether the lead content in an LNAPL plume is within the historical lead concentration ranges in gasolines. In addition to metals analyses, understanding of operational parameters such as the history of petroleum refining and handling operations, leaks, spills, and cleanup activities are needed for successful conclusion of the applicability of the petroleum exclusion.     

Effect of different types of clouds on surface UV-B and total solar irradiance at southern mid-latitudes: CMF determinations at Córdoba,Argentina

The effect of clouds on total and UV-B irradiance in Córdoba, Argentina, was studied employing the TUV 4.1 model and measurements obtained with YES UVB-1 and YES TSP-700 radiometers, and a spectral radiometer Ocean Optics USB-4000. The experimental measurements were selected from a 10 years dataset (1999–2008). Clouds were classified by direct observation as cirrus, cumulus, and stratocumulus. The broadband Cloud Modification Factors (CMFs) have been calculated in the range of the total and the UV-B radiation for these types of clouds. The relations between them were analyzed for a significant number of days. The broadband CMF values range from around 0.1 up to 1.25, depending on the wavelength interval and on the cloud type. The CMF_UVB versus CMF_T plots for different clouds have shown good adjustments and significant differences, which allows the distinction between them.Stratocumulus clouds show large attenuations and a linear relation with larger slopes as the solar zenith angle (SZA) increases. For this type of clouds an average slope of (1.0 ± 0.2) was found. The relation between the CMF for cumulus clouds is linear with an average slope of (0.61 ± 0.01). No dependence with the SZA was observed. Cirrus clouds plots show an exponential behavior with fit parameters equal to (0.48 ± 0.08) and (0.68 ± 0.15). However, when small SZA intervals are analyzed a linear relation is found. When the relations between the CMF were similar (cumulus and cirrus), the spectral variation in the UV range (320–420 nm) of a modified CMF (CMF_m) was used to distinguish them. Hence, the spectral differences among the three types of clouds have been also analyzed for several days and SZA. Here, it was found that the effect of cirrus is essentially wavelength independent while cumulus and stratocumulus clouds show exponential decay relations but with different ordinates.In the analyzed relations the microphysical properties of the clouds seem to determine its behavior while the optical thickness leads to the different degrees of attenuation.The results obtained in this work are in agreement with those found for other authors.     

The degradation of anilazine and dihydroxy‐anilazine at various soil depths of an orthic luvisol

Abstract

In conformity with Guideline 4.1 of the Federal German Biological Agency, degradation experiments with the fungicide active ingredient [benzene ring‐U‐¹⁴C]anilazine and its major metabolite [triazine ring‐U‐¹⁴C]dihydroxy‐anilazine were carried out in an orthic luvisol. Mineralization of the benzene ring carbon of anilazine amounted to less than 2 % in 110 days and that of the triazine ring carbon of dihydroxy‐anilazine to less than 8 %. Increasing the incubation temperature from 22 °C to 30 °C and adding organic substance influenced the mineralization slightly. In soils which received two or three applications in succeeding years with subsequent ageing in the open‐air lysimeter no stimulation of the mineralization was observed. Extractions after incubation showed that only 10.2 to 18.6 % of the ¹⁴C‐activity applied with anilazine was extractable with acetone/CaCl₂. The major proportion was bound in the fractions of the soil organic matter, namely 45.0 to 59.6 % of the radiocarbon applied was accounted for by the humin fraction, 12.0 to 27.4 % by the fulvic acids, and 9.4 to 15.0 % by the humic acids. In the case of dihydroxy‐anilazine, 28.9 to 89.7 % of the applied ¹⁴C‐activity was extractable with acetone/CaCl₂. Of tJhe radiocarbon bound in the soil, the greatest proportion, i.e. 18.5 to 35.5 % of the radiocarbon applied, was accounted for by the fulvic acids.     

Snow-pile and chamber experiments during the Polar Sunrise Experiment ‘Alert 2000’: exploration of nitrogen chemistry

Snow chamber and snow-pile experiments performed during the ‘Alert 2000’ campaign show significant release of NO, NO₂, and HONO in steady ratios under the influence of irradiation. Both light and a minimal degree of heating are required to produce this effect. We suggest diffusion and re-distribution of NO₃⁻ in the form of HNO₃ as an important step in the mechanism of active nitrogen release from the snowpack.     

Impact assessment of human diet changes with rapid urbanization on regional nitrogen and phosphorus flows—a case study of the megacity Shanghai

Regional material flows are strongly influenced by human diets. To diagnose and prevent environmental problems that threaten urban sustainability, the impact of human diet changes with rapid urbanization on the regional nitrogen (N) and phosphorus (P) flows were quantitatively evaluated. A survey of day-to-day activities was conducted of 450 individuals surveyed (adults over 18 years old) in three representative areas (the central district, the new district, and the suburban/rural areas) of Shanghai, a megacity which has attracted worldwide attention. The lifestyle (eating habits, domestic sanitation, drainage facilities, etc.) pattern was determined and the potential N and P loads from human diets on the environment were calculated. The daily potential nitrogen and phosphorus loads from human diets was 19.36 g-N, 1.80 g-P in the central district, 16.48 g-N, 1.52 g-P in the new district, and 13.04 g-N, 1.20 g-P in the suburban/rural areas of Shanghai. Respondents in all three areas, especially those in the suburban/rural areas reported a preference for increasing the intake of animal-derived as well as processed foods, which means that the potential N and P load from human diets to the environment will increase further. In addition, most respondents consider industrial wastewater discharge as the main cause of eutrophication of waterbodies, though in recent years water pollution caused by domestic wastewater has increased rapidly, but this has received much less attention. Environment-friendly eating habits and improvements in the environmental awareness will be required.     

Quantification of human adenovirus in irrigation water-soil-crop continuum: are consumers of wastewater-irrigated vegetables at risk?

Environmental Science and Pollution Research - Because of health concerns regarding the presence of enteric viruses in wastewater effluents, this study was designed to investigate the occurrence of...     

Assessing spatial variability of ambient nitrogen dioxide in Montréal, Canada, with a land-use regression model

The purpose of this study was to derive a land-use regression model to estimate on a geographical basis ambient concentrations of nitrogen dioxide (NO2) in Montreal, Quebec, Canada. These estimates of concentrations of NO2 will be subsequently used to assess exposure in epidemiologic studies on the health effects of traffic-related air pollution. In May 2003, NO2 was measured for 14 consecutive days at 67 sites across the city using Ogawa passive diffusion samplers. Concentrations ranged from 4.9 to 21.2 ppb (median 11.8 ppb). Linear regression analysis was used to assess the association between logarithmic concentrations of NO2 and land-use variables derived using the ESRI Arc 8 geographic information system. In univariate analyses, NO2 was negatively associated with the area of open space and positively associated with traffic count on nearest highway, the length of highways within any radius from 100 to 750 m, the length of major roads within 750 m, and population density within 2000 m. Industrial land-use and the length of minor roads showed-no association with NO2. In multiple regression analyses, distance from the nearest highway, traffic count on the nearest highway, length of highways and major roads within 100 m, and population density showed significant associations with NO2; the best-fitting regression model had a R2 of 0.54. These analyses confirm the value of land-use regression modeling to assign exposures in large-scale epidemiologic studies.     

Variations and its driven factors of anthropogenic nitrogen loads in the Yangtze River Economic Belt during 2000–2019

Environmental Science and Pollution Research - Since the millennium, China has economically taken off with rapid urbanization, and anthropogenic nitrogen emission intensity has undergone remarkable...