Assessment of uncertainties in a long range atmospheric transport model: Methodology, application and implications in a UK context

Acid deposition models are inherently simplified representations of real world behaviour and their performance is best evaluated by comparison with observations. National and international acid rain policy assessments handle observed and modelled deposition fields in different ways. Here, both the observed and modelled deposition fields are seen as uncertain and the Generalised Likelihood Uncertainty Estimation (GLUE) framework is used to choose acceptable sets of model input parameters that minimise the differences between them. These acceptable sets of model parameters are then used to estimate deposition budgets to the UK and to provide a probabilistic treatment of excess deposition over environmental quality standards (critical loads).     

In-stack emissions of heavy metals estimated by moss biomonitoring method and snow-pack analysis

Data from the chemical analysis of moss growing close to a thermal power station and snowpack have been used for the estimation of heavy metal deposition close to the point pollution sources. A semi-empirical model was proposed to describe atmospheric trace metal deposition close to the point pollution source. Model parameters were derived from experimental data, and nickel and vanadium quantities, washed out with snow and rain, were calculated. Using long-term meteorological observation data of rain and snow duration and metal uptake efficiencies in moss, the average emission rates of vanadium and nickel from the stack were calculated. The coincidence between data from emission inventory and model results was within 25%. It was estimated that in the vicinity of pollution source (within 30 km) about 15% out of total emitted metals were washed out by rain and snow events. Metal concentrations in the environment become indistinguishable from the background at a distance of about 20 km from the stack.     

Critical loads and steady-state chemistry for streams in the state of Maryland

The critical loads to streams, steady-state stream chemistry and catchment chemical weathering rate in 73 catchments has been determined in the state of Maryland, USA. It was calculated with the PROFILE model from chemical limits for biological indicators, soil mineralogy, soil texture, annual average temperature, average soil moisture, net long-term uptake of base cations and nitrogen to the vegetation, annual precipitation and runoff and deposition of sulphur and nitrogen precursors of acid deposition. The results show a full range of critical loads from very low values in the sensitive catchments of western Maryland and the Coastal Plain on the Chesapeake Bay, to insensitive catchments in the Fredrick Valley and Ridge and the Piedmont plain. The critical loads will be used as an input to an integrated regional assessment of the quantitative sensitivity of streams to acid rain, and the assessment of regional stream alkalinity response to different abatement strategies. The mapping of steady-state stream chemistry indicates that streams in Maryland are still acidfying under the present deposition load. Land-use seems to play an important role in maintaining neutral pH in many of the streams of Maryland.     

Reduction of atmospheric emissions due to switching from fuel oil to natural gas at a power plant in a critical area in Central Mexico

ABSTRACT

A case study was conducted to evaluate the SO₂ emission reduction in a power plant in Central Mexico, as a result of the shifting of fuel oil to natural gas. Emissions of criteria pollutants, greenhouse gases, organic and inorganic toxics were estimated based on a 2010 report of hourly fuel oil consumption at the “Francisco Pérez Ríos” power plant in Tula, Mexico. For SO₂, the dispersion of these emissions was assessed with the CALPUFF dispersion model. Emissions reductions of > 99% for SO₂, PM and Pb, as well as reductions >50% for organic and inorganic toxics were observed when simulating the use of natural gas. Maximum annual (993 µg/m³) and monthly average SO₂ concentrations were simulated during the cold-dry period (152–1063 µg/m³), and warm-dry period (239–432 µg/m³). Dispersion model results and those from Mexico City’s air quality forecasting system showed that SO₂ emissions from the power plant affect the north of Mexico City in the cold-dry period. The evaluation of model estimates with 24 hr SO₂ measured concentrations at Tepeji del Rio suggests that the combination of observations and dispersion models are useful in assessing the reduction of SO₂ emissions due to shifting in fuels. Being SO₂ a major precursor of acid rain, high transported sulfate concentrations are of concern and low pH values have been reported in the south of Mexico City, indicating that secondary SO₂ products emitted in the power plant can be transported to Mexico City under specific atmospheric conditions.

Implications: Although the surroundings of a power plant located north of Mexico City receives most of the direct SO₂ impact from fuel oil emissions, the plume is dispersed and advected to the Mexico City metropolitan area, where its secondary products may cause acid rain. The use of cleaner fuels may assure significant SO₂ reductions in the plant emissions and consequent acid rain presence in nearby populated cities and should be compulsory in critical areas to comply with annual emission limits and health standards.     

Atmospheric nitrogen deposition in south-east Scotland: Quantification of the organic nitrogen fraction in wet,dry and bulk deposition

Water soluble organic nitrogen (WSON) compounds are ubiquitous in precipitation and in the planetary boundary layer, and therefore are a potential source of bioavailable reactive nitrogen. This paper examines weekly rain data over a period of 22 months from June 2005 to March 2007 collected in 2 types of rain collector (bulk deposition and “dry + wet” deposition) located in a semi-rural area 15 km southwest of Edinburgh, UK (N55°51′44″, W3°12′19″). Bulk deposition collectors are denoted in this paper as “standard rain gauges”, and they are the design used in the UK national network for monitoring precipitation composition. “Dry + wet” deposition collectors are flushing rain gauges and they are equipped with a rain detector (conductivity array), a spray nozzle, a 2-way valve and two independent bottles to collect funnel washings (dry deposition) and true wet deposition. On average, for the 27 weekly samples with 3 valid replicates for the 2 types of collectors, dissolved organic nitrogen (DON) represented 23% of the total dissolved nitrogen (TDN) in bulk deposition. Dry deposition of particles and gas on the funnel surface, rather than rain, contributed over half of all N-containing species (inorganic and organic). Some discrepancies were found between bulk rain gauges and flushing rain gauges, for deposition of both TDN and DON, suggesting biological conversion and loss of inorganic N in the flushing samplers.     

Environmental tobacco smoke particles in multizone indoor environments

Environmental tobacco smoke (ETS) is a major source of human exposure to airborne particles. To better understand the factors that affect exposure, and to investigate the potential effectiveness of technical control measures, a series of experiments was conducted in a two-room test facility. Particle concentrations, size distributions, and airflow rates were measured during and after combustion of a cigarette. Experiments were varied to obtain information about the effects on exposure of smoker segregation, ventilation modification, and air filtration. The experimental data were used to test the performance of an analytical model of the two-zone environment and a numerical multizone aerosol dynamics model. A respiratory tract particle deposition model was also applied to the results to estimate the mass of ETS particles that would be deposited in the lungs of a nonsmoker exposed in either the smoking or nonsmoking room. Comparisons between the experimental data and model predictions showed good agreement. For time-averaged particle mass concentration, the average bias between model and experiments was less than 10%. The average absolute error was typically 35%, probably because of variability in particle emission rates from cigarettes. For the conditions tested, the use of a portable air filtration unit yielded 65–90% reductions in predicted lung deposition relative to the baseline scenario. The use of exhaust ventilation in the smoking room reduced predicted lung deposition in the nonsmoking room by more than 80%, as did segregating the smoker from nonsmokers with a closed door.     

Acidic and alkaline precipitation components in the mesoscale range under the aspect of meteorological factors and the emissions

At two sites in the north of the G.D.R. 80–100 km distant from industry rain from individual precipitation events was collected by automatic samplers and relevant ionic species were analyzed. The sampler is described.The cloud routes at the 850 hPa level were traced back 1 day and then seven sectors were formed for each collection site taking into consideration geographical aspects and features of the emission pattern for the rea concerned.Investigating the precipitation components as a function of the emission pattern knowledge of meteorological input parameters are required. The influence of these parameters is reported.Contrary to the combustion of other fossil fuels, in the case of brown coal combustion a considerable emission of neutralizing components (especially CaO) occurs, counteracting the formation of “acid rain”. This effect is clearly proven by means of individual examples and average considerations, i.e. the formation of acid rain does not only depend on the SO₂ and NO_x emissions.The wet deposition of all types of ions at the measuring site for every emission sector was calculated by means of precipitation statistics. Using these investigations reference points with regard to border crossing transport are given.     

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.     

Flow rates of ions in waters percolating through a model ecosystem with forest trees

From 1983-88 the long-term effects of low level exposure with O(3), SO(2) and simulated acid rain on mineral cycling in model ecosystems with spruce, fir and beech seedlings were investigated. Systems consisting of open-top chambers built above lysimeters were protected against the intrusion of ambient rain and dust. As part of the investigations on mineral cycling the fluxes of elements with water input and output of the canopy and soil compartments are presented. During the 5 year duration of the experiment, pronounced effects on canopy deposition and cation leaching were observed. Most noticeable were throughfall enrichment with sulfate through dry deposition of SO(2) as influenced by duration of needlewetting and factors promoting SO(2) oxidation. Depending on sulfur deposition, leaching of calcium, magnesium, manganese, zinc and ammonium from canopies was elevated, in total leading to enhanced soil input of acid. After 15 months, the water percolating the soils in the lysimeters of these treatments was acidified, with elevated flowrates of sulfate, manganese, calcium and magnesium. The results on canopy/soil leaching are compared to those from old conifer stands in the field.     

Two new ground-level cloud water sampler designs which reduce rain contamination

The ability to obtain discrete samples of cloud water for chemical analysis during periods when precipitation is occurring is important for studies of potential ecological effects of cloud and rain deposition. The advantage of the two cloud water collector designs presented, over others reported in the literature, is their ability to greatly reduce the entry of horizontally blown drizzle and rain droplets (> 200 μm) into the collector. The CWP Active Cloud Water Collector can be used in either stagnant or windy environments and requires 12 V battery power. The AMC/WPI Passive Cloud Water Collector is designed for windy environs and requires no power. Both collectors use removable cartridges with Teflon strands as a collection surface, and collect cloud droplets by inertial impaction. On Mount Washington, NH, the Active and Passive Cloud Water Collectors had an average cloud water collection rate of 1.8 and 1.5 ml min⁻¹, respectively.     

The organic precursors affecting the formation of disinfection by-products with chlorine dioxide

The object of this research was to study the formation of disinfection by-products by using chlorine dioxide (ClO2) as a disinfectant reacting with different properties of organic substance in natural aquatic environment. The adsorbent resin (XAD-4, XAD-7) was used to divide the organic matters in raw water into three groups. The influence of the function groups on structure, reaction tendency, and formation of disinfection by-products generated by the reaction of these organic substances with chlorine dioxide was explored. The experimental results show that the three different organic groups formed using adsorbent resin were hydrophobic substance, hydrophilic acid, and non-acid hydrophilics in proportions of 43%, 41%, and 16%, respectively. Within the raw water in our study, the hydrophilic substance had a higher distribution proportion than that described in general articles and journals, which indicates that this water was contaminated with pollution from human beings. The exploration of the reactivity of the three different organic substances with chlorine dioxide shows that the unit consumption of disinfection agent per unit organic matters (represented by ClO2/DOC) is in the following sequence hydrophobic substance > hydrophilic substance > non-acid hydrophilics. It indicated that larger molecular organic precursors had larger consumption of disinfectant. We also discovered that after the reaction of the three different organic substances with chlorine dioxide, the largest amount of disinfection by-products were generated by the non-acid hydrophilics.     

Effects of rhizobium, arbuscular mycorrhizal fungi and anion content of simulated rain on subterranean clover

An experiment was conducted to determine the extent to which rhizobia, mycorrhizal fungi, and anions in simulated rain affect plant growth response to acid deposition. Germinating subterranean clover seeds were planted in steam-pasteurized soil in pots and inoculated with Rhizobium leguminosarum, Glomus intraradices, Glomus etunicatum, R. leguminosarum + G. intraradices, R. leguminosarum + G. etunicatum, or no microbial symbionts. Beginning 3 weeks later, plants and the soil surface were exposed to simulated rain in a greenhouse on 3 days week(-1) for 12 weeks. Rain solutions were deionized water amended with background ions only (pH 5.0) or also adjusted to pH 3.0 with HNO3 only, H2SO4 only, or a 50/50 mixture of the two acids. Glomus intraradices colonized plant roots poorly, and G. intraradices-inoculated plants responded like nonmycorrhizal plants to rhizobia and rain treatments. Variation in plant biomass attributable to different rain formulations was strongest for G. etunicatum-inoculated plants, and the effect of rain formulation differed with respect to nodulation by rhizobia. The smallest plants at the end of the experiment were noninoculated plants exposed to rains (0.38 g mean dry weight total for 3 plants pot(-1)). Among nonnodulated plants infected by G. etunicatum, those exposed to HNO3 rain were largest, followed by plants exposed to HNO3 + H2SO4, pH 5.0, and H2SO4 rain, in that order. Among plants inoculated with both R. leguminosarum + G. etunicatum, however, the greatest biomass occurred with pH 5.0 rains, resulting in the largest plants in the study (1.00 g/3 plants). Treatment-related variation among root and shoot biomass data reflected those for whole-plant biomass. Based on quantification of biomass and N concentrations in shoot and root tissues, total N content of plants inoculated with G. etunicatum alone and exposed to the HNO3 + H2SO4 rains was approximately the same as plants inoculated with R. leguminosarum + G. entunicatum and exposed to pH 5 rains. Thus, the acid-mixture rains and rhizobia under no acid deposition provided approximately equal amounts of N in biomass. The significant interactions among rain formulation and the symbiotic status of the plants suggest that conclusions concerning the impact of acid deposition on plants in the environment cannot be considered reliable because most experiments on which such assessments are based have not tested confounding influences of microorganisms and precipitation characteristics.     

Importance of wet precipitation as a removal and transport process for atmospheric water soluble carbonyls

Carbonyl compounds exist in the atmosphere as either gases or aerosols. Some of them are water soluble and known as oxidation products of biogenic and/or anthropogenic hydrocarbons. Five carbonyl compounds, glyoxal (GO), 4-oxopentanal (4-OPA), glycolaldehyde (GA), hydroxyacetone (HA) and methylglyoxal (MG) have been identified in a temporal series of 12 rain samples. The concentrations of the compounds in the samples were high at the beginning of the rain event and decreased with time to relatively low and fairly constant levels, indicating that the compounds were washed out from the atmosphere at the start of the rain event. Possibly, these compounds also existed in the cloud condensation nuclei (CCN). Wet deposition rates of the carbonyl compounds were calculated for nine samples collected during a 20 h period. The deposition rates ranged from 0 (4-OPA) to 1.2×10⁻¹ mg C m⁻² h⁻¹ (MG) with the average of 2.9×10⁻² mg C m⁻² h⁻¹. Production rates of isoprene oxidation products (GA, HA and MG) in the area surrounding the sampling site were estimated with a chemical box model. The deposition rates exceeded the production rates in most samples. This indicates that the rainfall causes a large net flux of the water soluble compounds from the atmosphere to the ground. Insoluble carbonyl compounds such as n-nonanal and n-decanal were expected to be present in the atmosphere, but were not detected in the rain during the sampling period, suggesting that an aerosol containing these insoluble compounds does not effectively act as a CCN.     

Comparison of calculation models for wind-driven rain deposition on building facades

Wind-driven rain (WDR) is an important factor in the dry and wet deposition of atmospheric pollutants on building facades. In the past, different calculation models for WDR deposition on building facades have been developed and progressively improved. Today, the models that are most advanced and most frequently used are the semi-empirical model in the ISO Standard for WDR assessment (ISO), the semi-empirical model by Straube and Burnett (SB) and the CFD model by Choi. This paper compares the three models by applying them to four idealised buildings under steady-state conditions of wind and rain. In each case, the reference wind direction is perpendicular to the windward facade. For the CFD model, validation of wind-flow patterns and WDR deposition fluxes was performed in earlier studies. The CFD results are therefore considered as the reference case and the performance of the two semi-empirical models is evaluated by comparison with the CFD results based on two criteria: (1) ability to model the wind-blocking effect on the WDR coefficient; and (2) ability to model the variation of the WDR coefficient with horizontal rainfall intensity R_h. It is shown that both the ISO and SB model, as opposed to the CFD model, cannot reproduce the wind-blocking effect. The ISO model incorrectly provides WDR coefficients that are independent of R_h, while the SB model shows a dependency that is opposite to that by CFD. In addition, the SB model can provide very large overestimations of the WDR deposition fluxes at the top and side edges of buildings (up to more than a factor 5). The capabilities and deficiencies of the ISO and SB model, as identified in this paper, should be considered when applying these models for WDR deposition calculations. The results in this paper will be used for improvement and further development of these models.     

重庆酸雨对陆地生态系统的影响和控制对策——中日酸雨合作研究总结

中日合作研究项目：酸沉降对陆地生态系统的影响及其控制对策的研究,于１９９０至１９９５年期间在中国重庆地区进行。本文是该项目最终研究结果主要方面的报导,包括大气污染和酸雨的状况,酸沉降对池塘、森林和土壤生态系统的影响以及大气污染和酸雨控制对策。该项研究为今后酸沉降生态监测的研究,打下了有力的基础。     

Acid rain, storm period chemistry and their potential impact on stream communities in Hong Kong

Hong Kong experiences acid deposition, however, little is known about the potential impact upon aquatic ecosystems. In a small drainage basin observations reveal that despite acid rain runoff, both baseflow and stormflow, was close to neutral in terms of pH. During storm events chemical analysis reveals that calcium (Ca) concentrations tended to rise. It also appears that the input of acid rain may increase aluminium (Al) levels in the stream. Due to the increased levels of Ca and only slight changes in pH acid deposition may not be generating problems in this stream. The presence of mayflies reported elsewhere may further support the results of the chemical study.     

Bias correction of regional climate model simulations for the impact assessment of the climate change in Egypt

This study projected the future temperature change for Egypt during the late of this century (2071–2100) for three representative concentration pathways (RCP2.6, RCP4.5, and RCP8.5), by correcting regional climate model (RCM) simulations of average, maximum, and minimum daily temperature with reference to observed data of 26 stations. Four commonly used methods of bias correction have been applied and evaluated: linear scaling, variance scaling, and theoretical and empirical quantile mapping. The compromise programing results of the applied evaluation criteria show that the best method is the variance scaling, and thus it was applied to transfer the correction factor to the projections. All temperature indices are expected to increase significantly under all scenarios and reach the highest record by the end of the century, i.e., the expected increase in average, maximum, and minimum temperature ranges between 4.08–7.41 °C, 4.55–7.89 °C, and 3.88–7.23 °C, respectively. The largest temperature rise will occur in the summer, with the highest increase in the maximum (minimum) temperature of 10.9 °C (10 °C) in July and August under RCP8.5. The maximum (minimum) winter temperature, on the other hand, will drop by a maximum of 2 °C (1.35 °C) under RCP2.6. The Western Desert and Upper Egypt are the regions most affected by climate change, while the northern region of Egypt is the least affected. These findings would help in impact assessment and adaptation strategies and encourage further investigation to evaluate various climate models in order to obtain a comprehensive assessment of the climate change impacts on different hydrometeorological processes in Egypt.

     

Riparian Zone Influence on Stream Water Dissolved Organic Carbon Concentrations at the Swedish Integrated Monitoring Sites

Short-term variability in stream water dissolved organic carbon (DOC) concentrations is controlled by hydrology, climate and atmospheric deposition. Using the Riparian flow-concentration Integration Model (RIM), we evaluated factors controlling stream water DOC in the Swedish Integrated Monitoring (IM) catchments by separating out hydrological effects on stream DOC dynamics. Model residuals were correlated with climate and deposition-related drivers. DOC was most strongly correlated to water flow in the northern catchment (Gammtratten). The southern Aneboda and Kindla catchments had pronounced seasonal DOC signals, which correlated weakly to flow. DOC concentrations at Gårdsjön increased, potentially in response to declining acid deposition. Soil temperature correlated strongly with model residuals at all sites. Incorporating soil temperature in RIM improved model performance substantially (20–62% lower median absolute error). According to the simulations, the RIM conceptualization of riparian processes explains between 36% (Kindla) and 61% (Aneboda) of the DOC dynamics at the IM sites.     

Application of the nested grid STEM to an early summer acid rain in South Korea

The nested grid Sulfur Transport Eulerian Model (STEM) was developed and used to simulate the acid rain in Korea that occurred on 10 June 1996. The present nested grid system consists of three-grid systems. The coarsest grid system includes China, Korean Peninsula and Japan with the horizontal grid size of 80 km and the finest grid system includes only Korea with the horizontal grid size of 8.9 km. The calculated gas-phase SO₂ and O₃ concentrations agree relatively well with the field measurements. In addition, the model successfully reproduces the measured sulfate and nitrate concentrations in the rain water and futhermore identified the high concentration regions of liquid-phase sulfate and nitrate. In the present simulation conditions, most of the gas-phase of SO₂ and HNO₃ were washed out. A close relationship between wet deposition fluxes and precipitation rates were found for sulfate and nitrate. Finally, the model results also showed that a fine grid size is required to accurately calculate gas-phase concentrations as well as acid deposition fluxes.     

Different parameterisation of a Gaussian scheme: intercomparison study

The aim of this work is to define the most efficient parameterisation of the PBL (planetary boundary layer) by using the simulation with a simple Gaussian dispersion model of the plume type and comparing it with the improved OML model. A different type of σ_y and σ_z parameterisation in a Gaussian dispersion scheme was introduced. The old Pasquill–Gifford scheme and the new boundary layer parameterisation based on Monin–Obukhov length and other convective scaling parameters were compared, using a classical Gaussian model. For this comparison, the hourly average concentration and the long-term concentrations generated by these models, using same input data, were computed. These computed values and the field observations clearly show the importance of the parameterisations used by the models and the necessity of improving them. With this new parameterisation, we can easily add in new phenomena, such as dry and wet deposition, building effects and stack tip downwash penetration.