Observations and modelling of aerosol growth in marine stratocumulus—case study

Airborne measurements of the growth of the marine accumulation mode after multiple cycles through stratocumulus cloud are presented. The nss-sulphate cloud residual mode was log-normal in spectral shape and it’s mode radius was observed to progressively increase in size from 0.78 to 0.94 μm over 155 min of air parcel evolution through the cloudy marine boundary layer. The primary reason for this observed growth was thought to result from aqueous phase oxidation of SO₂ to aerosol sulphate in activated cloud drops. An aqueous phase aerosol–cloud-chemistry model was used to simulate this case study of aerosol growth and was able to closely reproduce the observed growth. The model simulations illustrate that aqueous phase oxidation of SO₂ in cloud droplets was able to provide enough additional sulphate mass to increase the size of activated aerosol. During a typical cloud cycle simulation, ≈4.6 nmoles kg^-1_air (0.44 μg m^-3) of sulphate mass was produced with ≈70% of sulphate production occurring in cloud droplets activated upon sea-salt nuclei and ≈30% occurring upon nss-sulphate nuclei, even though sea-salt nuclei contributed less than 15% to the activated droplet population. The high fraction of nss-sulphate mass internally mixed with sea-salt aerosol suggests that aqueous phase oxidation of SO₂ in cloud droplets activated upon sea-salt nuclei is the dominant nss-sulphate formation mechanism and that sea-salt aerosol provides the primary chemical sink for SO₂ in the cloudy marine boundary layer.     

Mercury and photochemistry in the marine boundary layer-modelling studies suggest the in situ production of reactive gas phase mercury

Following a modelling investigation of the role of the ambient aerosol in the cycling—that is the transport, transformation and deposition—of mercury in the atmosphere, the precise part played by the sea salt component of the marine aerosol in the remote marine boundary layer has been studied using a combination of models to describe the photolytic, gas phase and aqueous phase and heterogeneous chemistry of the marine boundary layer, in conjunction with inter phase mass transport and mercury chemistry. The role of the ocean in the emission of elemental mercury is, as yet, not entirely understood, but certainly the speciation of mercury deposited to the ocean surface is important as regards its re-emission. Models of mercury chemistry to date have tended to focus on cloud chemistry, and with good reason, as precipitation accounts for a large part of the global mercury deposition pattern; however, the composition of the marine aerosol is entirely different from that of cloud or fog droplets and the modelling studies here show that it plays a more local role being partially responsible for the gas phase speciation of mercury. The role of photochemical processes is investigated and particular attention is paid to halogen chemistry, as the chloride ion has been shown previously to have a notable effect on the concentration of oxidised mercury associated with particles, or better, solution droplets. The role of the sea salt component of the marine aerosol in the production of gas phase oxidised mercury species is described qualitatively and quantitatively.     

Non-dissipative cloud transport in Eulerian grid models by the volume-of-fluid (VOF) method

The formation of clouds is coupled to the vapour saturation condition. Cloud modelling is therefore dramatically disturbed by dilution processes, which are induced by recurrent interpolations on the fixed (Eulerian) grid. The numerical diffusion gives rise to degeneration and premature disappearance of the modelled clouds. The difficulties increase, if sectional mass representation in the drop microphysics and aerosol chemistry is considered. To tackle this problem, stringently defined and tracked phase boundaries are required.The numerical diffusion of clouds can be totally suppressed by the volume-of-fluid (VOF) method, which is applied here in connection with an atmospheric model. The cloud phase is distinguished by prognosing the partial cloud volume in all grid cells near the cloud boundary. Adopting elementary geometrical forms for the intracellular cloud volume and simple diagnostic rules of their alignment, the standard transport fluxes can be used in the new equation. Separate variables for the cloud and environmental phase complete the transport scheme.The VOF method and its realisation are described in detail. Advection, condensation, evaporation, and turbulent diffusion are considered within the VOF framework. The variation of the grid resolution and turbulence conditions for a rising thermal leads to striking arguments in favour of the VOF method, resulting in higher intensity, lifting, and lifetime as well as clear boundaries of the simulated clouds (even for low grid resolution).     

Halogen production from aqueous tropospheric particles

Box model studies have been performed to study the role of aqueous phase chemistry with regard to halogen activation for marine and urban clouds and the marine aerosol as well. Different chemical pathways leading to halogen activation in diluted cloud droplets and highly concentrated sea salt aerosol particles are investigated. The concentration of halides in cloud droplets is significantly smaller than in sea-salt particles, and hence different reaction sequences control the overall chemical conversions. In diluted droplets radical chemistry involving OH, NO(3), Cl/Cl(2)(-)/ClOH(-), and Br/Br(2)(-)/BrOH(-) gains in importance and pH independent pathways lead to the release of halogens from the particle phase whereas the chemistry in aerosol particles with high electrolyte concentrations is controlled by non-radical reactions at high ionic strengths and relatively low pH values.For the simulation of halogen activation in tropospheric clouds and aqueous aerosol particles in different environments a halogen module was developed including both gas and aqueous phase processes of halogen containing species. This module is coupled to a base mechanism consisting of RACM (Regional Atmospheric Chemistry Mechanism) and the Chemical Aqueous Phase Radical Mechanism CAPRAM 2.4 (MODAC-mechanism). Phase exchange is described by the resistance model by Chemistry of Multiphase Atmospheric Systems, NATO ASI Series, 1986.It can be shown that under cloud conditions the bromine atom is mainly produced by OH initiated reactions, i.e. its concentration maximum is reached at noon. In contrast, the concentration level of chlorine atoms is linked to NO(3) radical chemistry leading to a smaller amplitude between day and night time concentrations.The contribution of radical processes to halogen atom formation in the particle phase is evident, e.g. by halogen atoms which undergo direct phase transfer. Furthermore, the application of the multiphase model for initial concentrations for sea-salt aerosols shows that the particle phase can act as a main source of halogen containing molecules (Cl(2), BrCl, Br(2)) which are photolysed in the gas phase to yield halogen atoms (about 70% of all Cl sources and more than 99% for Br).     

Volcanic sulphate and arctic dust plumes over the North Atlantic Ocean

High time resolution aerosol mass spectrometry measurements were conducted during a field campaign at Mace Head Research Station, Ireland, in June 2007. Observations on one particular day of the campaign clearly indicated advection of aerosol from volcanoes and desert plains in Iceland which could be traced with NOAA Hysplit air mass back trajectories and satellite images. In conjunction with this event, elevated levels of sulphate and light absorbing particles were encountered at Mace Head. While sulphate concentration was continuously increasing, nitrate levels remained low indicating no significant contribution from anthropogenic pollutants. Sulphate concentration increased about 3.8 μg m⁻³ in comparison with the background conditions. Corresponding sulphur flux from volcanic emissions was estimated to about 0.3 TgS yr⁻¹, suggesting that a large amount of sulphur released from Icelandic volcanoes may be distributed over distances larger than 1000 km. Overall, our results corroborate that transport of volcanogenic sulphate and dust particles can significantly change the chemical composition, size distribution, and optical properties of aerosol over the North Atlantic Ocean and should be considered accordingly by regional climate models.     

Modelling changes of aerosol compositions over Belgium and Europe

Seasonal changes in aerosol compositions over Belgium and Europe are simulated with an extended version of the EUROS model. EUROS is capable of modelling mass and chemical composition of aerosols in two size fractions (PM_2.5 and PM_10-2.5). The chemical composition is expressed in terms of seven components: ammonium, nitrate, sulphate, primary inorganic compounds, elementary carbon, primary organic compounds and Secondary Organic Compounds (SOA). A comparison of modelled and measured aerosol concentrations showed that modelled concentrations are generally consistent with observed concentrations. The chemical composition of the aerosol showed a strong dependence on the season. High aerosol concentrations during the summer were mainly due to high concentrations of the secondary components nitrate, ammonium, sulphate and SOA in the size fraction PM_2.5. In contrast, during autumn and winter, increased PM-concentrations were mainly due to higher concentrations of primary components, especially in the size fraction PM_10-2.5.     

Sulphate aerosol size distributions at Mumbai,India, during the INDOEX-FFP (1998)

Sulphate size distributions were measured at the coastal station of Mumbai (formerly Bombay) through 1998, during the Indian ocean experiment (INDOEX) first field phase (FFP), to fill current gaps in size-resolved aerosol chemical composition data. The paper examines meteorological, seasonal and source-contribution effects on sulphate aerosol and discusses potential effects of sulphate on regional climate. Sulphate size-distributions were largely trimodal with a condensation mode (mass median aerodynamic diameter or MMAD 0.6 μm), a droplet mode (MMAD 1.9–2.4 μm) and a coarse mode (MMAD 5 μm). Condensation mode sulphate mass-fractions were highest in winter, consistent with the high meteorological potential for gas-to-particle conversion along with low relative humidity (RH). The droplet mode concentrations and MMADs were larger in the pre-monsoon and winter than in monsoon, implying sulphate predominance in larger sized particles within this mode. In these seasons the high RH, and consequently greater aerosol water in the droplet mode, would favour aerosol-phase partitioning and reactions of SO₂. Coarse mode sulphate concentrations were lowest in the monsoon, when continental contribution to sulphate was low and washout was efficient. In winter and pre-monsoon, coarse mode sulphate concentrations were somewhat higher, likely from SO₂ gas-to-particle conversion. Low daytime sulphate concentrations with a large coarse fraction, along with largely onshore winds, indicated marine aerosol predominance. High nighttime sulphate concentrations and a coincident large fine fraction indicated contributions from anthropogenic/industrial sources or from gas-to-particle conversion. Monthly mean sulphate concentrations increased with increasing SO₂ concentrations, RH and easterly wind direction, indicating the importance of gas-to-particle conversion and industrial sources located to the east. Atmospheric chemistry effects on sulphate size distributions in Mumbai, indicated by this data, must be further examined.     

Effect of topography on sulfate redistribution in cumulonimbus cloud development

An aqueous chemical module is created and included into a complex three-dimensional atmospheric cloud-resolving mesoscale model. In the chemical module, oxidation of S(IV) by ozone and hydrogen peroxide in cloud-water and rainwater, as important process of the sulfate production is included. To examine the impact of topography on the sulfate redistribution in a clean and a polluted environment, the complex topography of Serbia is included in the model. Numerical simulations of an isolated summer Cumulonimbus cloud shows that thunderstorms generate very strong vertical sulfate redistribution from the planetary boundary layer to the upper troposphere. This redistribution is sensitive to cloud dynamics, while cloud microphysics and precipitation determine wet removal of the chemical species. In simulations with realistic topography, the chemical species are transported over larger distances close to the surface, while in the upper atmosphere, there is no difference compared to the simulations without topography. The sensitivity tests of cloud chemistry to the physical processes are made. Omission of nucleation and impact scavenging of aerosols in the model simulations shows that 75.8 and 62.5 % of total sulfur mass deposited in the base experiment for the clean and the polluted environment, respectively, is the result of other processes. Exclusion of oxidation accounted for 19.2 and 37.7 % of total sulfur deposited for clean and polluted environment. Ignoring the ice phase almost not change mass of deposited sulfur: there is an increase of 2.9 and 1.5 % for clean and polluted atmosphere, respectively. Real topography conditions affect the sulfate redistribution in the sense of greater possibilities of transport. Numerical simulations without real topography give an artificial increase of deposited sulfur mass of about 25?30 %.     

Regional scale modelling of particulate matter in the UK,source attribution and an assessment of uncertainties

The models HARM and ELMO are used to investigate the importance of different source categories contributing to total PM₁₀ (SIA, SOA and primary particulate matter) across the UK and the impact of uncertainties on both present day and future concentration estimates. Modelled concentrations of SIA (secondary inorganic aerosol) are compared against data from the UK's Nitric Acid and Aerosol Network and SOA (secondary organic aerosol) against measurements made at the Bush Estate, Edinburgh. These data indicate that the HARM/ELMO modelling approach comes close to achieving mass closure. Comparison with national maps of total PM₁₀ indicate that the models underestimate particulate matter concentrations around large conurbations, probably due to the localised nature of emissions of primary particulates in these areas and model scale. The models are used to attribute particulate matter to different source and size categories, assessing the relative importance of primaries, SIA and SOA; the contributions of anthropogenic and biogenic precursors of SOA; the relative importance of PM_coarse (PM₁₀–PM_2.5) and PM_fine (PM_2.5) and UK vs. other EMEP area sources. The implications of these attributions for emissions control policies are discussed. The impact of uncertainties in emissions of the sources of primaries, SIA and SOA are explored. For primary PM₁₀ and SOA this has been achieved through emissions scaling and for SIA using the GLUE (Generalised Likelihood Uncertainty Estimation) approach. The selection of acceptable model parameter sets has been based on the need to retain the capability to model deposition of S and N species. The impact of uncertainty on estimates of present day SIA concentrations is illustrated for sites in the Nitric Acid and Aerosol Network. A more limited assessment for 2010 has been carried out at the national scale, illustrating that inclusion of uncertainty can change modelled concentrations from no exceedance of current air quality objectives, to one of exceedance over large areas of south and east England.     

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.     

A model study of smoke-haze influence on clouds and warm precipitation formation in Indonesia 1997/1998

In the last few decades, fire and smoke-haze occurrence increased in Indonesia by intentionally set land clearing fires and higher fire susceptibility of disturbed forests. Particularly, during El Niño years with prolonged droughts in Indonesia, land clearing fires become uncontrolled wildfires and produce large amounts of gaseous and particulate emissions. This paper investigates the influence of smoke-haze aerosols from such fires on clouds and precipitation over Indonesia during the El Niño event 1997/1998 by numerical modelling. Warm precipitation formation in both layered and convective clouds is calculated dependent on the atmospheric aerosol concentration. In the smoke-haze affected regions of Indonesia, aerosol–cloud interactions induce events with both precipitation suppression and increase compared to a reference simulation without aerosol–cloud interactions. The effect of precipitation suppression is found to dominate with about 2/3 of all precipitation modification events pointing to a prolongation of smoke-haze episodes. The corresponding convective cloud top height of shallow clouds is increased whereas distinct lower deep convective cloud top heights are found. The remaining about 1/3 events are characterised by increased precipitation and cloud liquid water content, accompanied by lower convective cloud top heights of shallow clouds and higher deep convective clouds.     

What are the sources and conditions responsible for exceedences of the 24 h PM10 limit value (50 μg m−3) at a heavily trafficked London site?

The European Union has set limit values for PM₁₀ to be met in 2005. At Marylebone Road, London, where the traffic is heavy, the daily limit value of 50 μg m⁻³ is exceeded more than 35 times a year. A total of 185 days with daily PM₁₀ concentrations exceeding the limit value of 50 μg m⁻³ measured between January 2002 and December 2004 (data capture of 89.5%) are discussed in this paper. These exceedences were more frequent in early spring and in autumn. Concentrations have been disaggregated into regional, urban (background) and local (street) contributions. Most of the episodes of gravimetric PM₁₀ above the limit value were associated with a high regional background and very often the regional contribution dominated the PM₁₀ mass. The secondary aerosol (especially the particulate nitrate) made a major contribution to the PM₁₀ load. These situations were frequently observed when air masses came from the European mainland (showing that both emissions from the UK and other EU countries contributed to the exceedences), and less frequently with maritime air masses that have stagnated over the UK (showing that emissions from the UK alone less frequently contributed to the high regional background). However, the higher frequency of episodes breaching the limit value at the roadside site than at the rural site and the higher frequency of PM₁₀ concentrations above the limit value on weekdays show that the high regional contributions are additional to local and urban emissions. Local emissions mainly due to traffic were the second important contributor to the exceedences, while the contribution of the urban background of London was less important than the local emissions and the regional background. Applying the pragmatic mass closure model of Harrison et al. [2003. A pragmatic mass closure model for airborne particulate matter at urban background and roadside sites. Atmospheric Environment 37, 4927–4933], revealed that the regional aerosol is comprised very largely of ammonium nitrate and sulphate and secondary organic aerosol. Findings suggest that international abatement of secondary aerosol precursors may be the most effective measure to fulfil the requirements of the European Directive 1999/30/CE by lowering the regional background.     

Validity and uncertainty in the calculation of an emission inventory for ammonia arising from agriculture in Great Britain

Emissions of ammonia have received increasing attention recently, following concern about the environmental consequences, especially in The Netherlands where levels are high due to intensive livestock farming. Direct local effects and more widespread consequences for a range of ecosystems have been attributed to ammonia emissions. As the most prevalent alkaline gas in the atmosphere, ammonia interacts with acidic species, changing their characteristics, chemical and physical behaviour, and enhancing their potential for acidification of soils. Ammonia also forms an important component of the nitrogen cycle and of nitrogen deposition. In the UK, as in many other European countries, there has been a considerable increase in the emission of ammonia within the last 30 years, estimated at about 50%. This results mainly from increases in agricultural production based on the steadily rising number of livestock and increasing fertilizer consumption. This paper discusses the various sources to emissions of ammonia from agricultural sources in the United Kingdom, and some of the uncertainties involved in constructing a national emissions inventory.     

Anthropogenic sulphate aerosol from India: estimates of burden and direct radiative forcing

A one-box chemical-meteorological model had been formulated to make preliminary estimates of sulphate aerosol formation and direct radiative forcing over India. Anthropogenic SO₂ emissions from India, from industrial fuel use and biomass burning, were estimated at 2.0 Tg S yr^-1 for 1990 in the range of previous estimates of 1.54 and 2.55 Tg S yr ^-1 for 1987. Meteorological parameters for 1990 from 18 Indian Meteorological Department stations were used to estimate spatial average sulphate burdens through formation from SO₂ reactions in gas and aqueous phase and removal by dry and wet deposition. The hydrogen peroxide reaction was found dominating for undepleted oxidant-rich conditions. Monthly mean sulphate burdens ranged from 2–10 mg m^-2 with a seasonal variation of winter–spring highs and summer lows in agreement with previous GCM studies. The sulphate burdens are dominated by sulphate removal rates by wet deposition, which are high in the monsoon period from June–November. Monthly mean direct radiative forcing from sulphate aerosols is high (−3.5 and −2.3 W m^-2) in December and January, is moderate (−1.3 to −1.5 W m^-2) during February to April and November and low (−0.4 to −0.6 W m^-2) during May to October also in general agreement with previous GCM estimates. This model, in reasonable agreement with detailed GCM results, gives us a simple tool to make preliminary estimates of sulphate burdens and direct radiative forcing.     

Chemistry and aerosols in the marine boundary layer: 1-D modelling of the three ACE-2 Lagrangian experiments

Three Lagrangian experiments were conducted during IGAC's second aerosol characterization experiment (ACE-2) in the area between Portugal, Tenerife and Madeira in June/July 1997. During each Lagrangian experiment, a boundary layer air mass was followed for about 30 h, and the temporal evolution of its chemical and aerosol composition was documented by a series of vertical profiles and horizontal box pattern flown by the Meteorological Research Flight research aircraft Hercules C130. The wealth of observational data that has been collected during these three Lagrangian experiments is the basis for the development and testing of a one-dimensional Lagrangian boundary layer model with coupled gas, aqueous, and aerosol phase chemistry. The focus of this paper is on current model limitations and strengths. We show that the model is able to represent the dynamical and chemical evolution of the marine boundary layer, in some cases requiring adjustments of the subsidence velocity and of the surface heat fluxes. Entrainment of a layer rich in ozone and carbon monoxide from a residual continental boundary layer into the marine boundary layer as well as in-cloud oxidation of sulphur dioxide by hydrogen peroxide are simulated, and coherent results are obtained, concerning the evolution of the small, presumably sulphate–ammonia aerosol mode.     

Modelling aerosol number distributions from a vehicle exhaust with an aerosol CFD model

Vehicular traffic contributes significantly to the aerosol number concentrations at the local scale by emitting primary soot particles and forming secondary nucleated nanoparticles. Because of their potential health effects, more attention is paid to the traffic induced aerosol number distributions.The aim of this work is to explain the phenomenology leading to the formation and the evolution of the aerosol number distributions in the vicinity of a vehicle exhaust using numerical modelling. The emissions are representative of those of a light-duty diesel truck without a diesel particle filter. The atmospheric flow is modelled with a computational fluid dynamics (CFD) code to describe the dispersion of pollutants at the local scale. The CFD code, coupled to a modal aerosol model (MAM) describing the aerosol dynamics, is used to model the tailpipe plume of a vehicle with emissions corresponding to urban driving conditions. On the basis of available measurements in Schauer et al. (1999), three surrogate species are chosen to treat the semi-volatile organic compounds in the emissions.The model simulates the formation of the aerosol distribution in the exhaust plume of a vehicle as follows. After emission to the atmosphere, particles are formed by nucleation of sulphuric acid and water vapour depending strongly on the thermodynamic state of the atmosphere and on the dilution conditions. The semi-volatile organic compounds are critical for the rapid growth of nanoparticles through condensation. The semi-volatile organic compounds are also important for the evolution of primary soot particles and can contribute substantially to their chemical composition.The most influential parameters for particle formation are the sulphur fuel content, the semi-volatile organic emissions and also the mass and initial diameter of the soot particles emitted. The model is able to take into account the complex competition between nucleation, condensation and dilution, as well as the interactions among the different aerosol modes. This type of model is a useful tool to better understand the dynamics leading to the formation of traffic induced aerosol distributions. However, some key issues such as the turbulence in the exhaust plume and in the wake of the car, the magnitude and chemical composition of semi-volatile organic emissions and the possible nucleation of organic species need to be investigated further to improve our understanding of ultrafine particle formation.     

A simple model which predicts some non-linear features between atmospheric sulphur and sulphur emissions

This paper develops a simple model and suggests a plausible chemico-physical mechanism for a non-linear response between atmospheric sulphur and sulphur emissions. It contains simplified representations of transport, deposition and conversion processes and uses a proxy in-cloud oxidant-limited reaction along a pathway connecting an emission source with a receptor site. Individual pathway responses to emissions show linear behaviour above a threshold. However, by averaging the values of SO2 at the receptor site from different pathways a continuous non-linear relationship is obtained. As emissions reduce, distant emission sources become less significant contributors of sulphur dioxide at a receptor site but their emissions are still counted in an emission inventory, leading to an apparent non-linearity. Sulphate is always found to contribute a signal to the receptor site total. This model goes someway to explaining a proposed 'crossover' between observed proportions of wet and dry deposited sulphur in the UK as emissions have been reduced.     

Dissolution of trace metals from lava ash: influence on the composition of rainwater in the Mount Etna volcanic area

Dissolution of trace metals from lava ash of the Mount Etna volcano in aqueous suspensions is studied as a function of solution pH and aerosol mass loading. The rate of dissolution and the final concentration increase with decreasing pH. Leaching experiments are found to be consistent with the observations of these metals in rainwater of the volcanic area. Elements such as Fe and Mn are important in the aqueous oxidation of SO(2) which increases the acidity of the rainwater. Leaching of Na, Ca, K, Fe and Mg may have a buffering effect in reacting with cloud and aerosol droplets.     

污泥热干化和燃烧特性试验研究

分别在桨叶式干化机和热重仪上进行污泥干化和燃烧试验,研究了污泥干化特性和污染物排放特性,并对污泥的燃烧特性进行分析。结果表明,污泥干化过程分为黏稠区、粘滞区和颗粒区3个阶段。干化过程排放的污染气体有氨气、氯化氢、氟化氢、氰化氢、甲烷和挥发性有机酸等,其中氨气为主要污染气体。经冷凝吸收和活性炭吸附处理后,各种污染气体浓度均显著降低,其中氨气去除率最高,达97.04%。污泥干化冷凝液的BOD5和COD质量浓度分别为4 040、8 510mg/L,氨氮的质量浓度为1 025mg/L,pH为9.84,属于高浓度有机废水。污泥的燃烧过程可以分为3个失重阶段:水分析出阶段(50～150℃),挥发分燃烧阶段(150～450℃),固定碳燃烧阶段(450～650℃)。分别用Kissinger法和Ozawa法计算挥发分燃烧阶段和固定碳燃烧阶段的活化能和动力学方程,挥发分燃烧阶段的活化能低于固定碳燃烧阶段,表明挥发分燃烧阶段污泥更易燃烧。污泥的燃烧过程在650℃时基本完成,因此实际工程应用中,设计干化污泥的焚烧温度在750℃比较合理。