Simulation results of global aerosol models have been assembled in the framework of the AeroCom intercomparison exercise. In this paper, we analyze the life cycles of dust, sea salt, sulfate, black carbon and particulate organic matter as simulated by sixteen global aerosol models. The differences among the results (model diversities) for sources and sinks, burdens, particle sizes, water uptakes, and spatial dispersals have been established. These diversities have large consequences for the calculated radiative forcing and the aerosol concentrations at the surface. Processes and parameters are identified which deserve further research. The AeroCom all-models-average emissions are dominated by the mass of sea salt (SS), followed by dust (DU), sulfate (SO 4 ), particulate organic matter (POM), and finally black carbon (BC). Interactive parameterizations of the emissions and contrasting particles sizes of SS and DU lead generally to higher diversities of these species, and for total aerosol. The lower diversity of the emissions of the fine aerosols, BC, POM, and SO 4 , is due to the use of similar emission inventories, and does therefore not necessarily indicate a better understanding of their sources. The diversity of SO 4 -sources is mainly caused by the disagreement on depositional loss of precursor gases and on chemical production. The diversities of the emissions are passed on to the burdens, but the latter are also strongly affected by the model-specific treatments of transport and aerosol processes. The burdens of dry masses decrease from largest to smallest: DU, SS, SO 4 , POM, and BC. The all-models-average residence time is shortest for SS with about half a day, followed by SO 4 and DU with four days, and POM and BC with six and seven days, respectively. The wet deposition rate is controlled by the solubility and increases from DU, BC, POM to SO 4 and SS. It is the dominant sink for SO 4 , BC, and POM, and contributes about one third to the total removal of SS and DU species. For SS and DU we find high diversities for the removal rate coefficients and deposition pathways. Models do neither agree on the split between wet and dry deposition, nor on that between sedimentation and other dry deposition processes. We diagnose an extremely high diversity for the uptake of ambient water vapor that influences the particle size and thus the sink rate coefficients. Furthermore, we find little agreement among the model results for the partitioning of wet removal into scavenging by convective and stratiform rain. Large differences exist for aerosol dispersal both in the vertical and in the horizontal direction. In some models, a minimum of total aerosol concentration is simulated at the surface. Aerosol dispersal is most pronounced for SO 4 and BC and lowest for SS. Diversities are higher for meridional than for vertical dispersal, they are similar for the individual species and highest for SS and DU. For these two components we do not find a correlation between vertical and meridional aerosol dispersal. In addition the degree of dispersals of SS and DU is not related to their residence times. SO 4 , BC, and POM, however, show increased meridional dispersal in models with larger vertical dispersal, and dispersal is larger for longer simulated residence times.

/pdf/analysis-and-quantification-of-the-diversities-of-aerosol-nam6kgi1wz.pdf

Analysis and quantification of the diversities of aerosol life cycles within AeroCom

This paper describes the development and evaluation of a new Model for Simulating Aerosol Interactions and Chemistry (MOSAIC), with a special focus on addressing the long-standing issues associated with solving the dynamic partitioning of semi-volatile inorganic gases (HNO3, HCl, and NH3) to size-distributed atmospheric aerosol particles. The coupled ordinary differential equations (ODE) for dynamic gas-particle mass transfer are extremely stiff, and the available numerical techniques are either too expensive or produce oscillatory and/or inaccurate steady-state solutions. These limitations are overcome in MOSAIC, which couples an accurate and computationally efficient thermodynamic module [Zaveri et al., 2005a,b] with a new dynamic gas-particle partitioning module described here. The algorithm involves time-split integrations of non-volatile and semi-volatile species, and a new concept of “dynamic pH” and an adaptive time-stepping scheme hold the key to smooth, accurate, and efficient solutions over the entire relative humidity range. MOSAIC is found to be in excellent agreement with a benchmark version of the model that uses LSODES (a Gear solver) for rigorously integrating the stiff ODEs. The steady-state MOSAIC results for monodisperse aerosol test cases are also in excellent agreement with those obtained with the benchmark equilibrium model AIM. MOSAIC is also evaluated within a 3-D model, andmore » the average CPU speed is estimated to be over 100 times faster than the dynamic aerosol model MADM [Pilinis et al., 2000]. These results suggest that MOSAIC is highly attractive for use in 3-D aerosol and air quality models in which both accuracy and efficiency are critically important.« less

https://agupubs.onlinelibrary.wiley.com/doi/pdf/10.1029/2007JD008782

Model for Simulating Aerosol Interactions and Chemistry (MOSAIC)

A review of atmospheric aerosol measurements

Analysis and abatement of air pollution involve a variety of technical disciplines. Formation of the most prevalent pollutants occurs during the combustion process, a tightly coupled system involving fluid flow, mass and energy transport, and chemical kinetics. Its complexity is exemplified by the fact that, in many respects, the simplest hydrocarbon combustion, the methane-oxygen flame, has been quantitatively modeled only within the last several years. Nonetheless, the development of combustion modifications aimed at minimizing the formation of the unwanted by-products of burning fuels requires an understanding of the combustion process. Fuel may be available in solid, liquid, or gaseous form; it may be mixed with the air ahead of time or only within the combustion chamber; the chamber itself may vary from the piston and cylinder arrangement in an automobile engine to a 10-story-high boiler in the largest power plant; the unwanted byproducts may remain as gases, or they may, upon cooling, form small particles. 

The only effective way to control air pollution is to prevent the release of pollutants at the source. Where pollutants are generated in combustion, modifications to the combustion process itself, for example in the manner in which the fuel and air are mixed, can be quite effective in reducing their formation. Most situations, whether a combustion or an industrial process, however, require some degree of treatment of the exhaust gases before they are released to the atmosphere. Such treatment can involve intimately contacting the effluent gases with liquids or solids capable of selectively removing gaseous pollutants or, in the case of particulate pollutants, directing the effluent flow through a device in which the particles are captured on surfaces. 

The study of the generation and control of air pollutants can be termed air pollution engineering and is the subject of this book. Our goal here is to present a rigorous and fundamental analysis of the production of air pollutants and their control. The book is intended for use at the senior or first-year graduate level in chemical, civil, environmental, and mechanical engineering curricula. We assume that the student has had basic first courses in thermodynamics, fluid mechanics, and heat transfer. The material treated in the book can serve as the subject of either a full-year or a one-term course, depending on the choice of topics covered. 

In the first chapter we introduce the concept of air pollution engineering and summarize those species classified as air pollutants. Chapter 1 also contains four appendices that present certain basic material that will be called upon later in the book. This material includes chemical kinetics, the basic equations of heat and mass transfer, and some elementary ideas from probability and turbulence. 

Chapter 2 is a basic treatment of combustion, including its chemistry and the role of mixing processes and flame structure. Building on the foundation laid in Chapter 2, we present in Chapter 3 a comprehensive analysis of the formation of gaseous pollutants in combustion. Continuing in this vein, Chapter 4 contains a thorough treatment of the internal combustion engine, including its principles of operation and the mechanisms of formation of pollutants therein. Control methods based on combustion modification are discussed in both Chapters 3 and 4. 

Particulate matter (aerosols) constitutes the second major category of air pollutants when classified on the basis of physical state. Chapter 5 is devoted to an introduction to aerosols and principles of aerosol behavior, including the mechanics of particles in flowing fluids, the migration of particles in external force fields, Brownian motion of small particles, size distributions, coagulation, and formation of new particles from the vapor by homogeneous nucleation. Chapter 6 then treats the formation of particles in combustion processes. 

Chapters 7 and 8 present the basic theories of the removal of particulate and gaseous pollutants, respectively, from effluent streams. We cover all the major air pollution control operations, such as gravitational and centrifugal deposition, electrostatic precipitation, filtration, wet scrubbing, gas absorption and adsorption, and chemical reaction methods. Our goal in these two chapters, above all, is to carefully derive the basic equations governing the design of the control methods. Limited attention is given to actual equipment specification, although with the material in Chapters 7 and 8 serving as a basis, one will be able to proceed to design handbooks for such specifications. 

Chapters 2 through 8 treat air pollution engineering from a process-by-process point of view. Chapter 9 views the air pollution control problem for an entire region or airshed. To comply with national ambient air quality standards that prescribe, on the basis of health effects, the maximum atmospheric concentration level to be attained in a region, it is necessary for the relevant governmental authority to specify the degree to which the emissions from each of the sources in the region must be controlled. Thus it is generally necessary to choose among many alternatives that may lead to the same total quantity of emission over the region. Chapter 9 establishes a framework by which an optimal air pollution control plan for an airshed may be determined. In short, we seek the least-cost combination of abatement measures that meets the necessary constraint that the total emissions not exceed those required to meet an ambient air quality standard. 

Once pollutants are released into the atmosphere, they are acted on by a variety of chemical and physical phenomena. The atmospheric chemistry and physics of air pollution is indeed a rich arena, encompassing the disciplines of chemistry, meteorology, fluid mechanics, and aerosol science. As noted above, the subject matter of the present book ends at the stack (or the tailpipe); those readers desiring a treatment of the atmospheric behavior of air pollutants are referred to J. H. Seinfeld, Atmospheric Chemistry and Physics of Air Pollution (Wiley-Interscience, New York, 1986). 

We wish to gratefully acknowledge David Huang, Carol Jones, Sonya Kreidenweis, Ranajit Sahu, and Ken Wolfenbarger for their assistance with calculations in the book.
Finally, to Christina Conti, our secretary and copy editor, who, more than anyone else, kept safe the beauty and precision of language as an effective means of communication, we owe an enormous debt of gratitude. She nurtured this book as her own; through those times when the task seemed unending, she was always there to make the road a little smoother. 

R. C. Flagan
J. H. Seinfeld

Fundamentals of Air Pollution Engineering

We analyzed size distributions measured continuously at a boreal forest measurement site at Hyytiala, Finland between 1996 and 2003. From the eight-year data we identified days when new aerosol particle formation was taking place as well as days when no formation was detected, removing days with ambiguous status. The event days were then classified based on whether it was possible to determine formation and growth rates of new particles. These characteristics were then calculated. We found that new particle formation happens frequently in the boreal forest boundary layer, with at least 24% of days containing an event. Events are more probable during spring and autumn than during other times of the year. The average formation rate of particles larger than 3 nm was 0.8 cm -3 s -1 , with enhanced rates during spring and autumn. The mean growth rate was 3.0 nm h -1 , peaking in summer. The created event database is valuable for future studies of reasons leading to new particle formation in the atmosphere.

Formation and growth of fresh atmospheric aerosols: eight years of aerosol size distribution data from SMEAR II, Hyytiälä, Finland

The processes leading to the formation of high-dispersed aerosols with particle size below 0.1 μ and the methods of generation and investigation of these aerosols are treated as well as their physical properties differing fundamentally from those of coarse aerosols. In spite of the great role played by high-dispersed aerosols in the important process of vapor condensation in space and their significance for many industries and meteorology, there are no monographs or reviews on this subject available in the literature, and the aim of the present work is to fill this gap.

A.G. Sutugin

Papers

Highly dispersed aerosols