Current Status of Air Quality Models for Particulate Matter

ABSTRACT

The current status of the mathematical modeling of atmospheric particulate matter (PM) is reviewed in this paper. Simulating PM requires treating various processes, including the formation of condensable species, the gas/ particle partitioning of condensable compounds, and in some cases, the evolution of the particle size distribution. The algorithms available to simulate these processes are reviewed and discussed. Eleven 3-dimensional (3-D) Eulerian air quality models for PM are reviewed in terms of their formulation and past applications. Results of past performance evaluations of 3-D Eulerian PM models are presented. Currently, 24-hr average PM_2.5 concentrations appear to be predicted within 50% for urban-scale domains. However, there are compensating errors among individual particulate species. The lowest errors tend to be associated with SO₄ ^2-, while NO₃ ^-, black carbon (BC), and organic carbon (OC) typically show larger errors due to uncertainties in emissions inventories and the prediction of the secondary OC fraction. Further improvements and performance evaluations are recommended.     

Application and Evaluation of Two Air Quality Models for Particulate Matter for a Southeastern U.S. Episode

Abstract

The Models-3 Community Multiscale Air Quality (CMAQ) Modeling System and the Particulate Matter Comprehensive Air Quality Model with extensions (PMCAMx) were applied to simulate the period June 29–July 10, 1999, of the Southern Oxidants Study episode with two nested horizontal grid sizes: a coarse resolution of 32 km and a fine resolution of 8 km. The predicted spatial variations of ozone (O₃), particulate matter with an aerodynamic diameter less than or equal to 2.5 μm (PM_2.5), and particulate matter with an aerodynamic diameter less than or equal to 10 μm (PM₁₀) by both models are similar in rural areas but differ from one another significantly over some urban/suburban areas in the eastern and southern United States, where PMCAMx tends to predict higher values of O₃ and PM than CMAQ. Both models tend to predict O₃ values that are higher than those observed. For observed O₃ values above 60 ppb, O₃ performance meets the U.S. Environmental Protection Agency's criteria for CMAQ with both grids and for PMCAMx with the fine grid only. It becomes unsatisfactory for PMCAMx and marginally satisfactory for CMAQ for observed O₃ values above 40 ppb.

Both models predict similar amounts of sulfate (SO₄ ^2?) and organic matter, and both predict SO₄ ^2? to be the largest contributor to PM_2.5. PMCAMx generally predicts higher amounts of ammonium (NH₄ ⁺), nitrate (NO₃ ^?), and black carbon (BC) than does CMAQ. PM performance for CMAQ is generally consistent with that of other PM models, whereas PMCAMx predicts higher concentrations of NO₃ ^?,NH₄ ⁺, and BC than observed, which degrades its performance. For PM₁₀ and PM_2.5 predictions over the southeastern U.S. domain, the ranges of mean normalized gross errors (MNGEs) and mean normalized bias are 37–43% and –33–4% for CMAQ and 50–59% and 7–30% for PMCAMx. Both models predict the largest MNGEs for NO₃ ^? (98–104% for CMAQ, 138–338% for PMCAMx). The inaccurate NO₃ ^? predictions by both models may be caused by the inaccuracies in the ammonia emission inventory and the uncertainties in the gas/particle partitioning under some conditions. In addition to these uncertainties, the significant PM overpredictions by PMCAMx may be attributed to the lack of wet removal for PM and a likely underprediction in the vertical mixing during the daytime.     

Modeling Atmospheric Mercury Deposition in the Vicinity of Power Plants

Abstract

Two mathematical models of the atmospheric fate and transport of mercury (Hg), an Eulerian grid–based model and a Gaussian plume model, are used to calculate the atmospheric deposition of Hg in the vicinity (i.e., within 50 km) of five coal–fired power plants. The former is applied using two different horizontal resolutions: coarse (84 km) and fine (16.7 km). More than 96% of the power plant Hg emissions are calculated with the plume model to be transported beyond 50 km from the plants. The grid–based model predicts a lower fraction to be transported beyond 50 km: >91% with a coarse resolution and >95% with a fine resolution. The contribution of the power plant emissions to total Hg deposition within a radius of 50 km from the plants is calculated to be <8% with the plume model, <14% with the Eulerian model with a coarse resolution, and <10% with the Eulerian model with a fine resolution. The Eulerian grid–based model predicts greater local impacts than the plume model because of artificially enhanced vertical dispersion; the former predicts about twice as much Hg deposition as the latter when the area considered is commensurate with the resolution of the grid–based model. If one compares the local impacts for an area that is significantly less than the grid–based model resolution, then the grid–based model may predict lower local deposition than the plume model, because two compensating errors affect the results obtained with the grid–based model: initial dilution of the power plant emissions within one or more grid cells and enhanced vertical mixing to the ground.     

Crushed concrete as a phosphate binding material: a potential new management tool

To avoid eutrophication of receiving waters, effective methods to remove P in urban and agricultural runoff are needed. Crushed concrete may be an effective filter material to remove dissolved and particulate P. Five types of crushed concrete were tested in the laboratory to evaluate the retention capacity of dissolved P. All types removed P very effectively (5.1-19.6 g P kg(-1) concrete), while the possible release of bound P varied between 0.4 and 4.6%. The retention rate was positively related to a decreasing concrete grain size due to an increasing surface area for binding. The P retention was also related to a marked increase in pH (up to pH 12), and the highest retention was observed when pH was high. Under these circumstances, column experiments showed outlet P concentrations <0.0075 mg P L(-1). Furthermore, experiments revealed that release of heavy metals is of no importance for the treated water. We demonstrate that crushed concrete can be an effective tool to remove P in urban and agricultural runoff as filter material in sedimentation/infiltration ponds provided that pH in the treated water is neutralized or the water is diluted before outlet to avoid undesired effects caused by the high pH.     

Vivianite precipitation and phosphate sorption following iron reduction in anoxic soils

Phosphorus retention in lowland soils depends on redox conditions. The aim of this study was to evaluate how the Fe(III) reduction degree affects phosphate adsorption and precipitation. Two similarly P-saturated, ferric Fe-rich lowland soils, a sandy and a peat soil, were incubated under anaerobic conditions. M?ssbauer spectroscopy demonstrated that Fe(III) in the sandy soil was present as goethite and phyllosilicates, whereas Fe(III) in the peat soil was mainly present as polynuclear, Fe-humic complexes. Following anoxic incubation, extensive formation of Fe(II) in the solids occurred. After 100 d, the Fe(II) production reached its maximum and 34% of the citrate-bicarbonate-dithionite extractable Fe (Fe(CBD)) was reduced to Fe(II) in the sandy soil. The peat soil showed a much faster reduction of Fe(III) and the maximum reduction of 89% of Fe(CBD) was reached after 200 d. Neoformation of a metavivianite/vivianite phase under anoxic conditions was identified by X-ray diffraction in the peat. The sandy soil exhibited small changes in the point of zero net sorption (EPC?) and P(i) desorption with increasing Fe(III) reduction, whereas in the peat soil P desorption increased from 80 to 3100 μmol kg?1 and EPC? increased from 1.7 to 83 μM, after 322 d of anoxic incubation. The fast Fe(III) reduction made the peat soils particularly vulnerable to changes in redox conditions. However, the precipitation of vivianite/metavivianite minerals may control soluble P(i) concentrations to between 2 and 3 μM in the long term if the soil is not disturbed.     

Evidence for Acidification-Driven Ecosystem Collapse of Danish Erica tetralix Wet Heathland

We report observations of disappearance of Erica tetralix in wet heathland, which is unlikely to be caused by competition, as E. tetralix is dying before its place is taken up by other species. To investigate the causes, we used both old and new data. Results showed that presence of Molinia caerulea and Calluna vulgaris were substantial in the former E. tetralix dominated areas. Measurements of the C/N ratio in the morlayer were between 21 and 26 under the E. tetralix stands. As the expected C/N ratio in a healthy nutrient poor ecosystem like the E. tetralix wet heathland is around 30, this indicates that the ratio is probably decreasing and, correspondingly, the probability of nitrogen leaching from the ecosystem is increasing. The morlayer pH was extremely low—between 3.03 and 3.78. This represents a pH decline since the 1960s, where pH values generally were above 4. This supports the hypothesis that the decrease in morlayer pH is the major factor explaining the disappearance of E. tetralix and that measures to increase pH should be considered as part of the recommendations for relevant future management.

Electronic supplementary material

The online version of this article (doi:10.1007/s13280-012-0251-z) contains supplementary material, which is available to authorized users.     

Treelines will be understood once the functional difference between a tree and a shrub is

Trees are taller than shrubs, grasses, and herbs. What is the disadvantage of being tall so that trees are restricted to warmer regions than low stature life forms? This article offers a brief review of the current state of biological treeline theory, and then explores the significance of tallness from a carbon balance, freezing resistance, and microclimatological perspective. It will be argued that having of a woody stem is neither a burden to the carbon balance nor does it add to the risk of freezing damage. The physiological means of trees to thrive in cold climates are similar to small stature plants, but due to their size, and, thus, closer aerodynamic coupling to air circulation, trees experience critically low temperatures at lower elevation and latitude than smaller plants. Hence, trees reach a limit at treeline for physical reasons related to their stature.     

Modeling Nutrient Transports and Exchanges of Nutrients Between Shallow Regions and the Open Baltic Sea in Present and Future Climate

We quantified horizontal transport patterns and the net exchange of nutrients between shallow regions and the open sea in the Baltic proper. A coupled biogeochemical-physical circulation model was used for transient simulations 1961-2100. The model was driven by regional downscaling of the IPCC climate change scenario A1B from two global General Circulation Models in combination with two nutrient load scenarios. Modeled nutrient transports followed mainly the large-scale internal water circulation and showed only small circulation changes in the future projections. The internal nutrient cycling and exchanges between shallow and deeper waters became intensified, and the internal removal of phosphorus became weaker in the warmer future climate. These effects counteracted the impact from nutrient load reductions according to the Baltic Sea Action Plan. The net effect of climate change and nutrient reductions was an increased net import of dissolved inorganic phosphorus to shallow areas in the Baltic proper.     

Impact of genetic diversity and inbreeding on the life-history of Chironomus midges over consecutive generations

We report results of a multigenerational experiment with Chironomus riparius. Two strains with a high and a low level of genetic variability were exposed to a low, environmentally relevant TBT concentration of 80 μg Sn kg⁻¹ sediment dw nominally (time weighted mean, based on measured concentrations: 4.5 μg Sn kg⁻¹ sediment dw), and various life history traits as well as genetic diversity were monitored for eleven consecutive generations. While TBT effects are hardly visible in the outbred and genetically diverse strain, the inbred and genetically impoverished strain shows a clearly reduced population growth rate compared to the control. Moreover, the impoverished strain shows an increase in fitness over time. Analyses of variation at five microsatellite loci revealed that the level of genetic variation is strongly reduced in the inbred compared to the outbred strain. Moreover, genetic diversity increases over time in the inbred strain. This finding explains the observed increase in fitness in both inbred lineages (control and TBT exposed). The results document that inbreeding and the level of genetic diversity might be of crucial importance in populations under pollution stress. Furthermore, ecotoxicological bioassays have to consider genetic diversity if results between laboratories should be comparable. Our data provides evidence that genetic diversity strongly contributes to the survival of a population exposed to chemical pollution.     

Blood serum concentrations of perfluorinated compounds in men from Greenlandic Inuit and European populations

Perfluorinated compounds (PFCs), such as perfluorooctane sulfonate (PFOS) and perfluorooctanoic acid (PFOA), are used in large quantities. They are persistent and found in measurable levels in human serum around the world. They have been associated with developmental, hepatic, and carcinogenic effects in animal studies. The aim of the present study was to describe levels of PFCs in serum among Inuits from Greenland and inhabitants from Warsaw, Poland and Kharkiv, Ukraine. Furthermore, the aim was to define social- and lifestyle related determinants of exposure for these compounds. Serum levels of seven PFCs were analyzed by liquid chromatography/tandem mass spectrometry (LC/MS/MS). The concentrations of PFOS and PFOA were the highest of all PFCs in all three populations with a total amount of almost 90% of the PFCs. The mean levels of PFOS and PFOA were in the Greenlandic Inuits 52 and 4.8 ng mL(-1), in Poland 19 and 5.2 ng mL(-1), and in Ukraine 8.1 and 1.9 ng mL(-1), respectively. Thus, levels of PFCs in the serum of Inuits on Greenland were among the highest described in a general population whereas the levels in Poland were similar to other industrialized countries. The exposure in Ukraine was rather low. In the Greenlandic Inuit population, intake of seafood, tea, age and area of living were significant determinants of PFOS concentrations and explained about 22% of the variation. For the other populations no strong determinants were found.