Critical loads and their exceedances at intensive forest monitoring sites in Europe

Intensive forest monitoring by means of harmonised methods has been conducted in Europe for more than a decade. Risks of atmospheric nitrogen and sulphur deposition are assessed by means of calculations of critical loads and their exceedances. In the present study throughfall and bulk deposition of nitrate (N-NO(3)), ammonium (N-NH(4)) and sulphate (S-SO(4)) show marked spatial patterns and temporal trends. In the period of observation (1999-2004), sulphate deposition on intensive monitoring plots decreased by about one quarter. This is in line with the reduction of S deposition by 70% since 1981 in Europe as a result of successful air pollution control politics under the Convention on Long-range Transboundary Air Pollution (CLRTAP). However, sulphate and especially nitrate and ammonium deposition were found to still exceed critical loads at many forest sites, indicating a continued need for further implementation of air pollution abatement strategies.     

Mapping of exceedances of ozone critical levels for crops and forest trees in The Netherlands: Preliminary results

Within the framework of the UN-ECE Convention on Long-Range Transboundary Air Pollution (CLRTAP) critical levels of ozone for forest trees and crops have been determined. In this paper procedures are presented for constructing maps of The Netherlands showing measured ozone concentrations for comparison with the critical levels. The critical ozone levels for forest trees and crops are exceeded widely and frequently in The Netherlands. The frequency and size of exceedances depend on meteorological conditions: during a hot, sunny summer like 1989 or 1990 exceedances of the critical levels by a factor of two or three were observed in the whole of The Netherlands; in a cold, rainy summer like 1991 or 1993 only minor exceedances were observed in some parts (mainly in the south) of the country.     

Evaluation of approaches to calculate critical metal loads for forest ecosystems

This paper evaluates approaches to calculate acceptable loads for metal deposition to forest ecosystems, distinguishing between critical loads, stand-still loads and target loads. We also evaluated the influence of including the biochemical metal cycle on the calculated loads. Differences are illustrated by examples of Cd, Cu, Pb and Zn for a deciduous forest on five major soil types in the Netherlands. Stand-still loads are generally lower than critical loads, which in turn are lower than the target loads indicating that present levels are below critical levels. Uncertainties in the calculated critical loads are mainly determined by the uncertainty in the critical limits and the chemical speciation model. Including the metal cycle has a small effect on the calculated critical loads. Results are discussed in view of the applicability of the critical load concept for metals in future protocols on the reduction in metal emissions.     

A conceptual framework: Redefining forest soil's critical acid loads under a changing climate

Federal agencies of several nations have or are currently developing guidelines for critical forest soil acid loads. These guidelines are used to establish regulations designed to maintain atmospheric acid inputs below levels shown to damage forests and streams. Traditionally, when the critical soil acid load exceeds the amount of acid that the ecosystem can absorb, it is believed to potentially impair forest health. The excess over the critical soil acid load is termed the exceedance, and the larger the exceedance, the greater the risk of ecosystem damage. This definition of critical soil acid load applies to exposure of the soil to a single, long-term pollutant (i.e., acidic deposition). However, ecosystems can be simultaneously under multiple ecosystem stresses and a single critical soil acid load level may not accurately reflect ecosystem health risk when subjected to multiple, episodic environmental stress. For example, the Appalachian Mountains of western North Carolina receive some of the highest rates of acidic deposition in the eastern United States, but these levels are considered to be below the critical acid load (CAL) that would cause forest damage. However, the area experienced a moderate three-year drought from 1999 to 2002, and in 2001 red spruce (Picea rubens Sarg.) trees in the area began to die in large numbers. The initial survey indicated that the affected trees were killed by the southern pine beetle (Dendroctonus frontalis Zimm.). This insect is not normally successful at colonizing these tree species because the trees produce large amounts of oleoresin that exclude the boring beetles. Subsequent investigations revealed that long-term acid deposition may have altered red spruce forest structure and function. There is some evidence that elevated acid deposition (particularly nitrogen) reduced tree water uptake potential, oleoresin production, and caused the trees to become more susceptible to insect colonization during the drought period. While the ecosystem was not in exceedance of the CAL, long-term nitrogen deposition pre-disposed the forest to other ecological stress. In combination, insects, drought, and nitrogen ultimately combined to cause the observed forest mortality. If any one of these factors were not present, the trees would likely not have died. This paper presents a conceptual framework of the ecosystem consequences of these interactions as well as limited plot level data to support this concept. Future assessments of the use of CAL studies need to account for multiple stress impacts to better understand ecosystem response.     

An empirical map of critical loads of acidity for soils in Great Britain

The method used to produce a critical load map of acidity for soils in Great Britain is described. Critical loads were assigned to the dominant soil in each 1 km grid square of the UK national grid. Mineral soils were assigned a critical load based on mineralogy and chemistry, using approaches appropriate to UK conditions. Critical loads for peat soils are based primarily on a maximum acceptable reduction of peat pH, and results from laboratory equilibration studies. The map shows that soils with small critical loads (<0.5 kmol_c ha⁻¹ year⁻¹) i.e. highly sensitive to acidic deposition, dominate in the north and west of Britain; the south and east are dominated by soils with large critical loads, with small areas of more sensitive soils associated with sandy soil-forming materials. A modified critical load map illustrates the potential impact of agricultural liming on soil critical loads.     

Assessment of the Nested Grid Model Estimates for Driving Regional Visibility Models in the Southwestern United States

ABSTRACT

The Nested Grid Model (NGM) is a primitive-equation meteorological model that is routinely exercised over North America for forecasting purposes by the National Meteorological Center. While prognostic meteorological models are being increasingly used to drive air quality models, their use in conducting annual simulations requires significant resources. NGM estimates of wind fields and other meteorological variables provide an attractive alternative since they are typically archived and readily available for an entire year. Preliminary evaluation of NGM winds during the summer of 1992 for application to the region surrounding the Grand Canyon National Park showed serious shortcomings. The NGM winds along the borders between California, Arizona and Mexico tend to be northwesterly with a speed of about 6 m/sec, while the observed flow is predominantly southerly at about 2-5 m/sec. The mesoscale effect of a thermal low pressure area over the highly heated Southern California and western Arizona deserts does not appear to be represented by the NGM because of its coarse resolution and the use of sparse observations in that region. Tracer simulations and statistical evaluation against special high resolution observations of winds in the southwest United States clearly demonstrate the northwest bias in NGM winds and its adverse effect on predictions of an air quality model. The “enhanced” NGM winds, in which selected wind observations are incorporated in the NGM winds using a diagnostic meteorological model provide additional confirmation on the primary cause of the northwest bias. This study has demonstrated that in situations where limited resources prevent the use of prognostic meteorological models, previously archived coarse resolution wind fields in which additional observations are incorporated to correct known biases provide an attractive option.     

Methodology for estimating soil carbon for the forest carbon budget model of the United States, 2001

The largest carbon (C) pool in United States forests is the soil C pool. We present methodology and soil C pool estimates used in the FORCARB model, which estimates and projects forest carbon budgets for the United States. The methodology balances knowledge, uncertainties, and ease of use. The estimates are calculated using the USDA Natural Resources Conservation Service STATSGO database, with soil dynamics following assumptions based on results of site-specific studies, and area estimates from the USDA Forest Service. Forest Inventory and Analysis data and national-level land cover data sets. Harvesting is assumed to have no effect on soil C. Land use change and forest type transitions affect soil C. We apply the methodology to the southeastern region of the United States as a case study.     

Spatial patterns of mobile source particulate matter emissions-to-exposure relationships across the United States

Assessing the public health benefits from air pollution control measures is assisted by understanding the relationship between mobile source emissions and subsequent fine particulate matter (PM_2.5) exposure. Since this relationship varies by location, we characterized its magnitude and geographic distribution using the intake fraction (iF) concept. We considered emissions of primary PM_2.5 as well as particle precursors SO₂ and NO_x from each of 3080 counties in the US. We modeled the relationship between these emissions and total US population exposure to PM_2.5, making use of a source–receptor matrix developed for health risk assessment. For primary PM_2.5, we found a median iF of 1.2 per million, with a range of 0.12–25. Half of the total exposure was reached by a median distance of 150 km from the county where mobile source emissions originated, though this spatial extent varied across counties from within the county borders to 1800 km away. For secondary ammonium sulfate from SO₂ emissions, the median iF was 0.41 per million (range: 0.050–10), versus 0.068 per million for secondary ammonium nitrate from NO_x emissions (range: 0.00092–1.3). The median distance to half of the total exposure was greater for secondary PM_2.5 (450 km for sulfate, 390 km for nitrate). Regression analyses using exhaustive population predictors explained much of the variation in primary PM_2.5 iF (R²=0.83) as well as secondary sulfate and nitrate iF (R²=0.74 and 0.60), with greater near-source contribution for primary than for secondary PM_2.5. We conclude that long-range dispersion models with coarse geographic resolution are appropriate for risk assessments of secondary PM_2.5 or primary PM_2.5 emitted from mobile sources in rural areas, but that more resolved dispersion models are warranted for primary PM_2.5 in urban areas due to the substantial contribution of near-source populations.     

Considerations of uncertainty in setting critical loads of acidity of soils: the role of weathering rate determination

The concept of critical loads has been generally accepted throughout Europe, and increasingly in Asian countries and the rest of the world, as providing the data which forms the basis for international negotiations on abatement strategies for emissions of acidifying pollutants. Central to the determination of quantitative critical loads of acidity for forests (and other ecosystems) is the rate at which the minerals in the soil weather or dissolve. Seven methods for determining these rates on a regional basis for the production of critical load maps have been suggested by the official bodies which are responsible for co-ordinating the European critical load mapping efforts. These methods are largely correlations which require a knowledge of the soil parent material and/or the soil mineralogy. The purpose of this paper is to review these weathering rate calculation methods and to assess whether it is currently possible to calculate numerically accurate critical loads for the production of regional critical load maps. A consideration of the data used to generate these methods and comparisons of the weathering rates calculated using various methods leads to the conclusion that at present it is not. Further work is needed to develop and maintain the initial credibility of critical loads both scientifically and as an aid to policy decisions.     

Methane emissions from 20 landfills across the United States using vertical radial plume mapping

Landfill fugitive methane emissions were quantified as a function of climate type and cover type at 20 landfills using U.S. Environmental Protection Agency (EPA) Other Test Method (OTM)-10 vertical radial plume mapping (VRPM) with tunable diode lasers (TDLs). The VRPM data were initially collected as g CH₄/sec emission rates and subsequently converted to g CH₄/m²/day rates using two recently published approaches. The first was based upon field tracer releases of methane or acetylene and multiple linear regression analysis (MLRM). The second was a virtual computer model that was based upon the Industrial Source Complex (ISC3) and Pasquill plume stability class models (PSCMs). Calculated emission results in g CH₄/m²/day for each measured VRPM with the two approaches agreed well (r ² = 0.93). The VRPM data were obtained from the working face, temporary soil, intermediate soil, and final soil or synthetic covers. The data show that methane emissions to the atmosphere are a function of climate and cover type. Humid subtropical climates exhibited the highest emissions for all cover types at 207, 127, 102, and 32 g CH₄/m²/day, for working face (no cover), temporary, intermediate, and final cover, respectively. Humid continental warm summers showed 67, 51, and 27 g CH₄/m²/day for temporary, intermediate, and final covers. Humid continental cool summers were 135, 40, and 26 g CH₄/m²/day for the working face, intermediate, and final covers. Mediterranean climates were examined for intermediate and final covers only and found to be 11 and 6 g CH₄/m²/day, respectively, whereas semiarid climates showed 85, 11, 3.7, and 2.7 g CH₄/m²/day for working face, temporary, intermediate, and final covers. A closed, synthetically capped landfill covered with soil and vegetation with a gas collection system in a humid continental warm summer climate gave mostly background methane readings and average emission rates of only 0.09 g CH₄/m²/day flux when measurable.

Implications The OTM-10 method is being proposed by EPA to quantify surface methane emissions from landfill covers. This study of 20 landfills across the United States was done to determine the efficacy of using OTM-10 for this purpose. Two recently published models were used to evaluate the methane flux results found with VRPM optical remote sensing. The results should provide a sense of the practicality of the method, its limitations at landfills, and the impact of climate upon the cover's methane flux. Measured field data may assist landfill owners in refining previously modeled methane emission factor default values.     

Methane emissions from 20 landfills across the United States using vertical radial plume mapping

Landfill fugitive methane emissions were quantified as a function of climate type and cover type at 20 landfills using US. Environmental Protection Agency (EPA) Other Test Method (OTM)-10 vertical radial plume mapping (VRPM) with tunable diode lasers (TDLs). The VRPM data were initially collected as g CH4/sec emission rates and subsequently converted to g CH4/m2/ day rates using two recently published approaches. The first was based upon field tracer releases of methane or acetylene and multiple linear regression analysis (MLRM). The second was a virtual computer model that was based upon the Industrial Source Complex (ISC3) and Pasquill plume stability class models (PSCMs). Calculated emission results in g CH4/m2/day for each measured VRPM with the two approaches agreed well (r2 = 0.93). The VRPM data were obtained from the working face, temporary soil, intermediate soil, and final soil or synthetic covers. The data show that methane emissions to the atmosphere are a function of climate and cover type. Humid subtropical climates exhibited the highest emissions for all cover types at 207, 127, 102, and 32 g CH4/m2/day, for working face (no cover), temporary, intermediate, and final cover, respectively. Humid continental warm summers showed 67, 51, and 27 g CH4/m2/day for temporary, intermediate, and final covers. Humid continental cool summers were 135, 40, and 26 g CH4/m2/day for the working face, intermediate, and final covers. Mediterranean climates were examined for intermediate and final covers only and found to be 11 and 6 g CH4/m2/day, respectively, whereas semiarid climates showed 85, 11, 3.7, and 2.7 g CH4/m2/day for working face, temporary, intermediate, and final covers. A closed, synthetically capped landfill covered with soil and vegetation with a gas collection system in a humid continental warm summer climate gave mostly background methane readings and average emission rates of only 0.09 g CH4/m2/day flux when measurable.     

Trends in speciated fine particulate matter and visibility across monitoring networks in the Southeastern United States

Trends in fine particulate matter <2.5 microm in diameter (PM2.5) and visibility in the Southeastern United States were evaluated for sites in the Interagency Monitoring of Protected Visual Environments, Speciated Trends Network, and Southeastern Aerosol Research and Characterization Study networks. These analyses are part of the technical assessment by Visibility Improvement-State and Tribal Association of the Southeast (VISTAS), the regional planning organization for the southeastern states, in support of State Implementation Plans for the regional haze rule. At all of the VISTAS IMPROVE sites, ammonium sulfate and organic carbon (OC) are the largest and second largest contributors, respectively, to light extinction on both the 20% haziest and 20% clearest days. Ammonium nitrate, elemental carbon (EC), soils, and coarse particles make comparatively small contributions to PM2.5 mass and light extinction on most days at the Class I areas. At Southern Appalachian sites, the 20% haziest days occur primarily in the late spring to fall, whereas at coastal sites, the 20% haziest days can occur through out the year. Levels of ammonium sulfate in Class I areas are similar to those in nearby urban areas and are generally higher at the interior sites than the coastal sites. Concentrations of OC, ammonium nitrate, and, sometimes, EC, tend to be higher in the urban areas than in nearby Class I areas, although differences in measurement methods complicate comparisons between networks. Results support regional controls of sulfur dioxide for both regional haze and PM2.5 implementation and suggest that controls of local sources of OC, EC, or nitrogen oxides might also be considered for urban areas that are not attaining the annual National Ambient Air Quality Standard for PM2.5.     

Assessing the risk of N leaching from forest soils across a steep N deposition gradient in Sweden

Nitrogen leaching from boreal and temporal forests, where normally most of the nitrogen is retained, has the potential to increase acidification of soil and water and eutrophication of the Baltic Sea. In parts of Sweden, where the nitrogen deposition has been intermediate to high during recent decades, there are indications that the soils are close to nitrogen saturation. In this study, four different approaches were used to assess the risk of nitrogen leaching from forest soils in different parts of Sweden. Nitrate concentrations in soil water and C:N ratios in the humus layer where interpreted, together with model results from mass balance calculations and detailed dynamic modelling. All four approaches pointed at a risk of nitrogen leaching from forest soils in southern Sweden. However, there was a substantial variation on a local scale. Basing the assessment on four different approaches makes the assessment robust.     

Regional visibility modeling for the Eastern United States

Visibility modeling over long transport distances is complicated not only by the chemical and removal processes, but also by the multiplicity of sources from different areas that contribute to the particle and gaseous concentrations—and visibility impairment—at specific locations. To study interregional pollutant exchanges and their effect on visibility, a regional model has been developed and applied to the eastern United States and the visibility reduction budgeted according to area of origin. The new model, called VISMAP-1, produces short-term (three-hour) and long-term (monthly) sulfate concentrations; visibility calculations are made by applying a mass-to-light-scattering function to the aerosol concentrations. This function is weighted according to relative humidity to account for hygroscopic particle growth. One of the most useful features of this model is its capability to budget fine-particulate and gaseous concentrations in various receptor regions according to the contribution of source regions.In this analysis for visibility effects, three-hour SURE (Sulfate Regional Experiment) sulfate measurements for July 1978 are compared to fine-particle calculations to evaluate the model's ability to predict the transport of aerosol sulfur for the shorter averaging period. Visibility is modeled from the sulfate calculations using an empirical mass-to-light-scattering function. This technique is commonly used to determine aerosol light-scattering properties at given relative humidities. National Weather Service visual range observations have been compared with the model's visibility calculations; both regional patterns of visibility degradation and the absolute magnitude of the reduction in visual range are evaluated. Preliminary results are encouraging and the VISMAP modeling approach appears to be a useful step toward identifying long-range source/receptor relationships that affect visibility.     

Surface ozone at four remote island sites and the preliminary assessment of the exceedances of its critical level in Japan

Analysis of the recent surface ozone data at four remote islands (Rishiri, Oki, Okinawa, and Ogasawara) in Japan indicates that East Asian anthropogenic emissions significantly influence the boundary layer ozone in Japan. Due to these regional-scale emissions, an increase of ozone concentration is observed during fall, winter, and spring when anthropogenically enhanced continental air masses from Siberia/Eurasia arrive at the sites. The O₃ concentrations in the “regionally polluted” continental outflow among sites are as high as 41–46 ppb in winter and 54–61 ppb in spring. Meanwhile, marine air masses from the Pacific Ocean show as low as 13–14 ppb of O₃ at Okinawa and Ogasawara in summer but higher O₃ concentrations, 24–27 ppb, are observed at Oki and Rishiri due to the additional pollution mainly from Japan mainland. The preliminary analysis of the exceedances of ozone critical level using AOT40 and SUM06 exposure indices indicates that the O₃ threshold were exceeded variously among sites and years. The highest AOT40 and SUM06 were observed at Oki in central Japan where the critical levels are distinctly exceeded. In the other years, the O₃ exposures at Oki, Okinawa, and Rishiri are about or slightly higher than the critical levels. The potential risk of crop yields reduction from high level of O₃ exposure in Japan might not be a serious issue during 1990s and at present because the traditional growing season in Japan are during the low O₃ period in summer. However, increases of anthropogenic emission in East Asia could aggravate the situation in the very near future.     

A statistical approach to the regional use of critical loads

The premise of this paper is that: (1) effects of spatial heterogeneity of watershed response to acid deposition must be considered when models are used to set abatement policies, and (2) the evaluation of critical chemical values is a better measure off the effects of abatement policies than the comparison of deposition values to critical loads. The authors used Monte Carlo methods to apply a site-specific version of the RAINS-Lake-Model to a regional data set from The Netherlands. Statistical methods were then used to identify the important parameters affecting the spatial and temporal response, i.e. a change in pH, of watersheds to acid deposition and a subset of sensitive and insensitive watersheds were derived. The results show that the failure to subset a region into sensitive and insensitive zones may result in an erroneous estimation of the effect of abatement policies based on critical loads alone.     

Direct damage to vegetation caused by acid rain and polluted cloud: definition of critical levels for forest trees

The concept of critical levels was developed in order to define short-term and long-term average concentrations of gaseous pollutants above which plants may be damaged. Although the usual way in which pollutants in precipitation (wet deposition) influence vegetation is by affecting soil processes, plant foliage exposed to fog and cloud, which often contain much greater concentrations of pollutant ions than rain, may be damaged directly. The idea of a critical level has been extended to define concentrations of pollutants in wet deposition above which direct damage to plants is likely. Concentrations of acidity and sulphate measured in mountain and coastal cloud are summarised. Vegetation at risk of injury is identified as montane forest growing close to the cloud base, where ion concentrations are highest. The direct effects of acidic precipitation on trees are reviewed, based on experimental exposure of plants to simulated acidic rain, fog or mist. Although most experiments have reported results in terms of pH (H(+) concentration), the accompanying anion is important, with sulphate being more damaging than nitrate. Both conifers and broadleaved tree seedlings showing subtle changes in the structural characteristics of leaf surfaces after exposure to mist or rain at or about pH 3.5, or sulphate concentration of 150 micromol litre(-1). Visible lesions on leaf surfaces occur at around pH 3 (500 micromol litre(-1) sulphate), broadleaved species tending to be more sensitive than conifers. Effects on photosynthesis and water relations, and interactions with other stresses (e.g. frost), have usually been observed only for treatments which have also caused visible injury to the leaf surface. Few experiments on the direct effects of polluted cloud have been conducted under field conditions with mature trees, which unlike seedlings in controlled conditions, may suffer a growth reduction in the absence of visible injury. Although leaching of cations (Ca(2+), Mg(2+), K(+)) is stimulated by acidic precipitation, amounts leached are small compared with root uptake, unless soils have been impoverished. This aspect of the potential effects of acidic precipitation is best considered in terms of the long-term critical-load of pollutants to the soil. Given the practical difficulties in monitoring cloud water composition, a method for defining critical levels is proposed, which uses climatological average data to identify the duration and frequency of hill cloud, and combines this information with measured or modelled concentrations of particulate sulphate in the atmosphere, to derive cloud water concentrations as a function of cloud liquid water content. For forests within 100 m of the cloud base the critical levels of particulate sulphate, corresponding to solution concentrations in the range 150-500 micromol litre(-1), are in the range 1-3.3 microg S m(-3). These concentrations are observed over much of central Europe, suggesting that many montane forests are at risk of direct effects of fossil-fuel-derived pollutants in cloud.     

Estimates of ambient background concentrations of trace metals in soils for risk assessment

Site-specific or soil type-specific ambient background concentrations (ABCs) of trace metals in soils are needed for risk assessment. We investigated three different methods for estimating ABCs in soils using a dataset of 5691 soil samples from England and Wales. The concentrations of Co, Cr and Ni were strongly associated with Al and Fe, and multiple regressions explained 62-85% of their variation, and Al and Fe can therefore be used to predict ABCs for these metals. Soil texture had a major influence on the concentrations of Cd, Co, Cr, Cu, Ni and Zn, and the medians were 3-5 fold higher in clayey than in sandy soils. This was used to predict texture-specific ABCs. Lead concentration was higher in acidic peaty soils than in other soils. A probability graph method was used to estimate ABC for Pb in a population of relatively uncontaminated soils. Potential applications of ABCs are discussed.     

Trends in atmospheric reactive nitrogen for the Eastern United States

Reactive nitrogen can travel far from emission sources and impact sensitive ecosystems. From 2002 to 2006, policy actions have led to decreases in NO(x) emissions from power plants and motor vehicles. In this study, atmospheric chemical transport modeling demonstrates that these emissions reductions have led to a downward trend in ambient measurements of transported reactive nitrogen, especially atmospheric concentrations and wet deposition of nitrate. The trend in reduced nitrogen, namely ammonium, is ambiguous. As reduced nitrogen becomes a larger fraction of the reactive nitrogen budget, wide-spread NH(3) measurements and improved NH(3) emissions assessments are a critical need.