Evidence of sulphur and nitrogen deposition signals at the United Kingdom Acid Waters Monitoring Network sites

Some recent studies of trends in sulphate in surface waters have alluded to possible lag effects imposed by catchment soils, resulting in discrepancies between trends in deposition and run-off. To assess the extent of these possible effects in the UK, sulphate concentration data from the United Kingdom Acid Waters Monitoring Network (AWMN) sites are compared with estimates of sulphur deposition at each site. From these data, input-output budgets are computed at an annual time scale. The estimated budgets suggest a close association between catchment sulphur inputs and outputs at an annual scale, with well-balanced annual budgets at most sites, indicative of only minor lag effects. A similar analysis of the AWMN site nitrogen budget shows little evidence of an association between nitrogen inputs and outputs at this time scale.     

Modelling the spatial distribution of SO2 and NOx emissions in Ireland

The spatial distributions of sulphur dioxide (SO2) and nitrogen oxides (NOx) emissions are essential inputs to models of atmospheric transport and deposition. Information of this type is required for international negotiations on emission reduction through the critical load approach. High-resolution emission maps for the Republic of Ireland have been created using emission totals and a geographical information system, supported by surrogate statistics and landcover information. Data have been subsequently allocated to the EMEP 50 x 50-km grid, used in long-range transport models for the investigation of transboundary air pollution. Approximately two-thirds of SO2 emissions in Ireland emanate from two grid-squares. Over 50% of total SO2 emissions originate from one grid-square in the west of Ireland, where the largest point sources of SO2 are located. Approximately 15% of the total SO2 emissions originate from the grid-square containing Dublin. SO2 emission densities for the remaining areas are very low, < 1 t km-2 year-1 for most grid-squares. NOx emissions show a very similar distribution pattern. However, NOx emissions are more evenly spread over the country, as about 40% of total NOx emissions originate from road transport.     

Modelling the formation and atmospheric transport of secondary inorganic aerosols with special attention to regions with high ammonia emissions

Regional simulations of sulfate, nitrate and ammonium aerosols were performed by a nested application of the online-coupled three-dimensional Eulerian model system COSMO-MUSCAT. This was done in a domain covering the northern part of Germany and surrounding regions for the full month of May and a 6-week period in August/September 2006 with the primary focus on secondary inorganic aerosol levels caused by ammonia emissions from domesticated animals and agricultural operations.The results show that in situations with westerly winds ammonium nitrate dominates with concentrations of about 5–10 μg m^?3 whereas the ammonium sulfate concentrations are about 5 μg m^?3. In situations with winds mainly from the East characterized by warmer and dryer air the ammonium sulfate concentrations have their maximum at about 10 μg m^?3 whereas at the same time no ammonium nitrate is present.A reduction of agricultural NH₃ emissions by 50% in a regional scale reduces the ammonium nitrate concentrations to a maximum of 30%, while the ammonium sulfate concentrations are unchanged. The reduction of NH₃ emissions in a more limited area (here in the Federal state of Germany Niedersachsen) does have no noticeable effect neither on ammonium sulfate nor on ammonium nitrate.     

Variability of SO2, CO,and light hydrocarbons over a megacity in Eastern India: effects of emissions and transport

The Indo-Gangetic plain (IGP) has received extensive attention of the global scientific community due to higher levels of trace gases and aerosols over this region. Satellite retrievals and model simulations show that, in particular, the eastern part IGP is highly polluted. Despite this attention, in situ measurements of trace gases are very limited over this region. This paper presents measurements of SO₂, CO, CH₄, and C₂–C₅ NMHCs during March 2012–February 2013 over Kolkata, a megacity in the eastern IGP, with a focus on processes impacting their levels. The mean SO₂ and C₂H₆ concentrations during winter and post-monsoon periods were eight and three times higher compared to pre-monsoon and monsoon. Early morning enhancements in SO₂ and several NMHCs during winter connote boundary layer effects. Daytime elevations in SO₂ during pre-monsoon and monsoon suggest impacts of photo-oxidation. Inter-species correlations and trajectory analysis evince transport of SO₂ from regional combustion sources (e.g., coal burning in power plants, industries) along the east of the Indo-Gangetic plain impacting SO₂ levels at the site. However, C₂H₂ to CO ratio over Kolkata, which are comparable to other urban regions in India, show impacts of local biofuel combustions. Further, high levels of C₃H₈ and C₄H₁₀ evince the dominance of LPG/petrochemicals over the study location. The suite of trace gases measured during this study helps to decipher between impacts of local emissions and influence of transport on their levels.     

Response of needle sulphur and nitrogen concentrations of Scots pine versus Norway spruce to SO2 and NO2

The results of two field studies and an open-top chamber fumigation experiment showed that the response of mature Scots pine to SO(2) and NO(2) differed from that of mature Norway spruce. Moreover, the response of pine seedlings to SO(2) and NO(2) differed from that of mature trees. The greater increase in the needle total S concentrations of pine suggested more abundant stomatal uptake of SO(2) compared to spruce. Both pine seedlings and mature trees also seemed to absorb more N from atmospheric deposition. Mature pine was able to assimilate SO(4)(2-) derived from SO(2) into organic S more effectively than mature spruce at the high S and N deposition sites, whereas both pine and spruce seedlings accumulated SO(4)-S under NO(2)+SO(2) exposure. Spruce, in turn, accumulated SO(4)-S even when well supplied with N. Net assimilation of SO(4)(2-) in conifer seedlings was enhanced markedly by elevated temperature. To protect the northern coniferous forests against the harmful effects of S and N deposition, it is recommended that the critical level for SO(2) as a growing season mean be set at 5-10 microg m(-3) and NO(2) at 10-15 microg m(-3), depending on the 'effective temperature sum' and/or whether SO(2) and NO(2) occur alone or in combination.     

Effects of reduced nitrogen and sulphur deposition on the water chemistry of moorland pools

To assess changes as a result of reduced acidifying deposition, water chemistry data from 68 Dutch moorland pools were collected during the periods 1983-1984 and 2000-2006. Partial recovery was observed: nitrate- and ammonium-N, sulphur and aluminium concentrations decreased, while pH and alkalinity increased. Calcium and magnesium concentrations decreased. These trends were supported by long term monitoring data (1978-2006) of four pools. Increased pH correlated with increases in ortho-phosphate and turbidity, the latter due to stronger coloration by organic acids. Increased ortho-phosphate and turbidity are probably the result of stronger decomposition of organic sediments due to decreased acidification and may hamper full recovery of moorland pool communities. In addition to meeting emission targets for NO_x, NH_x and SO_x, restoration measures are still required to facilitate and accelerate recovery of acidified moorland pools.     

Modeling the atmospheric transport and deposition of polychlorinated dibenzo-p-dioxins and dibenzofurans in North America

The atmospheric fate of polychlorinated dibenzo-p-dioxins (PCDDs) and polychlorinated dibenzofurans (PCDFs) was simulated for the year 2000 in North America using a SMOKE/CMAQ-based chemical transport model that was modified for this purpose. The 1999 USEPA emission inventories of PCDD/Fs and criteria pollutants were used. The 1995 Canadian emission inventory of criteria pollutants and the 1995 Canadian area source emissions for PCDD/Fs were used with the 2000 Canadian point source emissions. Modifications to CMAQ involved coupling it with dual organic matter (OM) absorption and black carbon (BC) adsorption models to calculate PCDD/F gas–particle partitioning. The model satisfactorily reproduced the particle bound fractions at all rural sites for which there were measured data and across the whole domain, the modeled vs. measured differences in particle bound fractions were less than 20% for nearly all congeners. The model predicted ambient air PCDD/F concentrations were also consistent with measurements. Simulated deposition fluxes were within 58% of direct measurements. PCDD/F atmospheric depositions to each of the Great Lakes were estimated for the year 2000. The results indicate that approximately 76% of the total deposition of PCDD/Fs to the Great Lakes (in W-TEQ, or toxic equivalent units as defined by the World Health Organization) is attributed to PCDD/Fs absorbed into OM in aerosol. For all of the lakes, more than 92% of all deposition is particle phase wet deposition and only 5–8% is particle phase dry deposition. Wet deposition from the gas phase is negligible. Of the 17 toxic PCDD/F congeners, the Cl_4–5DD/F compounds contribute approximately 70% to the total atmospheric deposition to the Great Lakes. The seasonal changes in the PCDD/F deposition flux track variations in ambient temperature.     

PAHs in background soils from Western Europe: influence of atmospheric deposition and soil organic matter

The levels and distribution of polynuclear aromatic hydrocarbons (PAHs) were determined in soil samples from background locations in the UK and Norway, to investigate their spatial distribution and the controlling environmental factors. Concentrations ranged between 42 and 11200 microg kg(-1) (geometric mean 640 microg kg(-1)) and 8.6 and 1050 microg kg(-1) (150 microg kg(-1)) dry weight in the UK and Norwegian soil, respectively. Proximity to sources and locations susceptible to high atmospheric depositional inputs resulted in higher concentrations. Statistically significant relationships were observed between PAH and total organic carbon (TOC) in the Norwegian samples. High molecular weight PAHs correlated with black carbon (BC) in UK-woodland soil. These observations support the hypothesis that TOC plays an important role in the retention of PAHs in soil and that PAHs are often combined with BC during combustion emissions. PAHs with 4 and more rings comprised approximately 90% of total PAHs in the UK soil, but only 50% in the Norwegian soil. The mixture of PAHs implied that fractionation occurred during long-range atmospheric transport and deposition. The lighter PAHs with lower K(ow) values more readily reached the most remote sites. The heavier PAHs with higher K(ow) values remained in closer proximity to sources.     

Regional and historical variation in the nitrogen content of Racomitrium lanuginosum in Britain in relation to atmospheric nitrogen deposition

The moss Racomitrium lanuginosum (Hedw.) Brid. is an important component of the drier parts of ombrotrophic mires and montane heaths in north-western Britain. The extent and quality of the montane heaths dominated by R. lanuginosum has declined in recent decades, perhaps in part due to the effects of acidic deposition at high elevations. This paper examines the effect of atmospheric nitrogen deposition, which has increased during this century, on the nitrogen content of R. lanuginosum in Britain. The nitrogen content of the moss reflects the magnitude of the atmospheric supply being least in north-western Scotland and greatest (as much as six-fold greater) near to urban centres in northern England. This regional difference was less marked (only approx. two-fold) during the 19th century (as revealed from the analysis of herbarium specimens) when nitrogen concentrations were appreciably lower. Transplant studies both between regions and between sites within a mountain system demonstrated the importance of atmospheric deposition in determining the tissue nitrogen concentration of the moss. The results are discussed in relation to the potential importance of the enhanced atmospheric nitrogen supply to the normally nitrogen-impoverished montane heaths, and to the growth and persistence of the moss.     

Observed trends in ambient concentrations of C2–C8 hydrocarbons in the United Kingdom over the period from 1993 to 2004

Hourly measurements of up to 26 C₂–C₈ hydrocarbons have been made at eight urban background sites, three urban-industrial sites, a kerbside and a rural site in the UK from 1993 onwards up until the end of December 2004. Average annual mean benzene and 1,3-butadiene concentrations at urban background locations have declined at about −20% per year and the observed declines have exactly mimicked the inferred declines in benzene and 1,3-butadiene emissions over the same period. Ninety-day rolling mean concentrations of ethylene, propylene, n- and i-butane, n- and i-pentane, isoprene and propane at urban and rural sites have also declined steadily by between −10% and −30% per year. Rolling mean concentrations of acetylene, 2- and 3-methylpentane, n-hexane, n-heptane, cis- and trans-but-2-ene, cis- and trans-pent-2-ene, toluene, ethylbenzene and o-, m- and p-xylene at a roadside location in London have all declined at between −14% and −21% per year. These declines demonstrate that motor vehicle exhaust catalysts and evaporative canisters have effectively and efficiently controlled vehicular emissions of hydrocarbons in the UK. Urban ethane concentrations arising largely from natural gas leakage have remained largely unchanged over this same period.     

The role of mechanical and biological treatment in reducing methane emissions from landfill disposal of municipal solid waste in the United Kingdom

In Europe, the European Union Landfill Directive aims to reduce the negative environmental impacts of landfilling. This is mainly to be achieved by reducing the quantity of organic matter deposited, through measures such as the separate collection and recycling of the organic waste stream or pretreatment of residual wastes before landfilling. Other than incineration or other thermal processes, mechanical biological treatment is playing an increasingly important role. This study was conducted to seek the benefits of municipal solid waste (MSW) pretreatment, as well as the differences in methane production from the landfilling of untreated and mechanically/biologically treated (MBT) MSW using GasSim simulation. Results demonstrated that methane production rates vary significantly among waste fractions. Those that contribute most to methane generation (organic material and potentially reusable or recyclable material) could be targeted and treated before landfilling. The statistic relationship from the first phase of the study indicated that to match the increasingly stringent landfill waste organic content allowance, local councils should prioritize the reduction/sorting of certain targeted fractions, such as paper, card, green waste, and other putrescibles from MSW. Moreover, mechanical treatment alone produces organic-rich waste called mechanically sorted organic residues (MSORs), which can be viewed as an organic content concentration process. Mechanically and biologically pretreated waste, on the other hand, differs significantly from untreated MSW and MSORs. This work demonstrated that if efficient mechanical-biological treatment is used, considerable reductions in biological activity, landfill gas production, and energy content/total organic carbon could be achieved. Using GasSim, reductions in methane production of >74% have been simulated if a 90% organic content reduction can be achieved during biological treatment on MSORs. A 50-60% organic content reduction by following biological treatment can turn MSOR properties only into normal MSW equivalent though considerably less volume.     

Effects of geographical location and land use on atmospheric deposition of nitrogen in the State of Connecticut

A network of eight monitoring stations was established to study the atmospheric nitrogen concentration and deposition in the State of Connecticut. The stations were classified into urban, rural, coastal and inland categories to represent the geographical location and land use characteristics surrounding the monitoring sites. Nitrogen species including nitrate, ammonium, nitric acid vapor and organic nitrogen in the air and precipitation were collected, analyzed and used to infer nitrogen concentrations and dry and wet deposition flux densities for the sampling period from 1997 through 1999, with independently collected meteorological data. Statistical analyses were conducted to evaluate the spatial variations of atmospheric concentration and deposition fluxes of total nitrogen in Connecticut. A slightly higher atmospheric concentration of total nitrogen was observed along the Connecticut coastline of Long Island Sound compared to inland areas, while the differences of nitrogen deposition fluxes were insignificant between coastal and inland sites. The land use characteristics surrounding the monitoring sites had profound effects on the atmospheric nitrogen concentration and dry deposition flux. The ambient nitrogen concentration over the four urban sites was averaged 38.9% higher than that over the rural sites, resulting a 58.0% higher dry deposition flux in these sites compared to their rural counterparts. The local industrial activities and traffic emissions of nitrogen at urban areas had significant effects on the spatial distribution of atmospheric nitrogen concentration and dry deposition flux in the State. Wet and total deposition fluxes appeared to be invariant between the monitoring sites, except for high flux densities measured at Old Greenwich, a monitoring station near to and downwind of the New York and New Jersey industrial complexes.     

Broadband UV spectroscopy system used for monitoring of SO2 and NO emissions from thermal power plants

A gas monitoring system based on broadband absorption spectroscopic techniques in the ultraviolet region is described and tested. The system was employed in real-time continuous concentration measurements of sulfur dioxide (SO₂) and nitric oxide (NO) from a 220-ton h^?1 circulating fluidized bed (CFB) boiler in Shandong province, China. The emission coefficients (per kg of coal and per kWh of electricity) and the total emission of the two pollutant gases were evaluated. The measurement results showed that the emission concentrations of SO₂ and NO from the CFB boiler fluctuated in the range of 750–1300 mg m^?3 and 100–220 mg m^?3, respectively. Compared with the specified emission standards of air pollutants from thermal power plants in China, the values were generally higher for SO₂ and lower for NO. The relatively high emission concentrations of SO₂ were found to mainly depend on the sulfur content of the fuel and the poor desulfurization efficiency. This study indicates that the broadband UV spectroscopy system is suitable for industrial emission monitoring and pollution control.     

Expected ozone benefits of reducing nitrogen oxide (NOx) emissions from coal-fired electricity generating units in the eastern United States

On hot summer days in the eastern United States, electricity demand rises, mainly because of increased use of air conditioning. Power plants must provide this additional energy, emitting additional pollutants when meteorological conditions are primed for poor air quality. To evaluate the impact of summertime NO_x emissions from coal-fired electricity generating units (EGUs) on surface ozone formation, we performed a series of sensitivity modeling forecast scenarios utilizing EPA 2018 version 6.0 emissions (2011 base year) and CMAQ v5.0.2. Coal-fired EGU NO_x emissions were adjusted to match the lowest NO_x rates observed during the ozone seasons (April 1–October 31) of 2005–2012 (Scenario A), where ozone decreased by 3–4 ppb in affected areas. When compared to the highest emissions rates during the same time period (Scenario B), ozone increased ～4–7 ppb. NO_x emission rates adjusted to match the observed rates from 2011 (Scenario C) increased ozone by ～4–5 ppb. Finally in Scenario D, the impact of additional NO_x reductions was determined by assuming installation of selective catalytic reduction (SCR) controls on all units lacking postcombustion controls; this decreased ozone by an additional 2–4 ppb relative to Scenario A. Following the announcement of a stricter 8-hour ozone standard, this analysis outlines a strategy that would help bring coastal areas in the mid-Atlantic region closer to attainment, and would also provide profound benefits for upwind states where most of the regional EGU NO_x originates, even if additional capital investments are not made (Scenario A).

Implications: With the 8-hr maximum ozone National Ambient Air Quality Standard (NAAQS) decreasing from 75 to 70 ppb, modeling results indicate that use of postcombustion controls on coal-fired power plants in 2018 could help keep regions in attainment. By operating already existing nitrogen oxide (NO_x) removal devices to their full potential, ozone could be significantly curtailed, achieving ozone reductions by up to 5 ppb in areas around the source of emission and immediately downwind. Ozone improvements are also significant (1–2 ppb) for areas affected by cross-state transport, especially Mid-Atlantic coast regions that had struggled to meet the 75 ppb standard.     

Estimates of emissions of SO2, NOx, HCl and NH3 from a densely populated region of the UK

Estimates of emissions of SO2, NOx, HCl and NH3 have been made for a densely populated region of the UK, the North-West of England, using data on power generation, incinerator plant capacity, fuel usage and animal and human population statistics. The spatial distributions of SO2 and NOx emissions are quite different, reflecting their different source strengths. The emissions from motor vehicles make up 52% of the NOx emissions from the North-West of England, whilst those from fossil-fuel-fired power stations make up 20%. The emissions of fossil-fuel-fired power stations make up 58% of SO2 emissions from the North-West. A large fossil-fuel-fired power station is the largest known point source for emissions of SO2, NOx and HCl. The largest contribution to NH3 emissions in the North-West is from cattle. Humans may contribute some NH3 to overall emissions but there is considerable uncertainty as to how much is emitted and what fraction of this is deposited within buildings. The uncertainties in the methodologies used are high-lighted and, where possible, recommendations are made as to how future emissions estimates might be improved. Potential reductions in emissions of SO2, NOx and HCl are discussed under basic scenarios of planned power station closures in the area and the compliance of the electricity generation industry with the European Community Directive on Large Combustion Plants.     

The effects of atmospheric nitrogen deposition in the Rocky Mountains of Colorado and southern Wyoming, USA-a critical review

The Rocky Mountains of Colorado and southern Wyoming receive atmospheric nitrogen (N) deposition that ranges from 2 to 7 kg ha(-1) yr(-1), and some previous research indicates pronounced ecosystem effects at the highest rates of deposition. This paper provides a critical review of previously published studies on the effects of atmospheric N deposition in the region. Plant community changes have been demonstrated through N fertilization studies, however, N limitation is still widely reported in alpine tundra and subalpine forests of the Front Range, and sensitivity to changes in snow cover alone indicate the importance of climate sensitivity in these ecosystems. Retention of N in atmospheric wet deposition is <50% in some watersheds east of the Continental Divide, which reflects low biomass and a short growing season relative to the timing and N load in deposition. Regional upward temporal trends in surface water NO(3)(-) concentrations have not been demonstrated, and future trend analyses must consider the role of climate as well as N deposition. Relatively high rates of atmospheric N deposition east of the Divide may have altered nutrient limitation of phytoplankton, species composition of diatoms, and amphibian populations, but most of these effects have been inconclusive to date, and additional studies are needed to confirm hypothesized cause and effect relations. Projected future population growth and energy use in Colorado and the west increase the likelihood that the subtle effects of atmospheric N deposition now evident in the Front Range will become more pronounced and widespread in the future.     

An integrative analysis of the role of atmospheric deposition and land management practices on nitrogen in the US agricultural sector

Additions of anthropogenic nitrogen (N) compounds constitute one of the major classes of air pollutants of significance to human health and the environment. Reliance on wet deposition measurements alone can lead to considerable underestimates (by 40-60%) of the total (wet + dry) atmospheric N deposition. In addition, wet deposition of N are about 20% of the levels that are lost due to volatilization (primarily ammonia). Nevertheless, in the agricultural sectors of the Mississippi River basins, farm management practices, and recycling of N within cropping systems clearly outweigh the contributions of atmospheric deposition. As opposed to native vegetation and forests, there are no records of the negative effects of atmospheric N deposition on crop yield. Similarly, field studies on the interactions of atmospheric N compounds with the incidence and spread of pathogens does not permit any generalizations. Nitrogen applied as fertilizer affects disease probably more by its effect on the plant growth than by its effects on pathogens. In contrast, atmospheric nitrogen dioxide appears to be a stimulant of aphid performance. Under conditions of heavy weed infestation, N fertilization stimulates weed growth and competitiveness, rather than crop yield.     

Modeling analyses of the effects of changes in nitrogen oxides emissions from the electric power sector on ozone levels in the eastern United States

In this paper, we examine the changes in ambient ozone concentrations simulated by the Community Multiscale Air Quality (CMAQ) model for summer 2002 under three different nitrogen oxides (NOx) emission scenarios. Two emission scenarios represent best estimates of 2002 and 2004 emissions; they allow assessment of the impact of the NOx emissions reductions imposed on the utility sector by the NOx State Implementation Plan (SIP) Call. The third scenario represents a hypothetical rendering of what NOx emissions would have been in 2002 if no emission controls had been imposed on the utility sector. Examination of the modeled median and 95th percentile daily maximum 8-hr average ozone concentrations reveals that median ozone levels estimated for the 2004 emission scenario were less than those modeled for 2002 in the region most affected by the NOx SIP Call. Comparison of the "no-control" with the "2002" scenario revealed that ozone concentrations would have been much higher in much of the eastern United States if the utility sector had not implemented NOx emission controls; exceptions occurred in the immediate vicinity of major point sources where increased NO titration tends to lower ozone levels.