Aerosols are of central importance for atmospheric chemistry and physics, the biosphere, climate, and public health. The airborne solid and liquid particles in the nanometer to micrometer size range ...influence the energy balance of the Earth, the hydrological cycle, atmospheric circulation, and the abundance of greenhouse and reactive trace gases. Moreover, they play important roles in the reproduction of biological organisms and can cause or enhance diseases. The primary parameters that determine the environmental and health effects of aerosol particles are their concentration, size, structure, and chemical composition. These parameters, however, are spatially and temporally highly variable. The quantification and identification of biological particles and carbonaceous components of fine particulate matter in the air (organic compounds and black or elemental carbon, respectively) represent demanding analytical challenges. This Review outlines the current state of knowledge, major open questions, and research perspectives on the properties and interactions of atmospheric aerosols and their effects on climate and human health.
An esthetic example of the wide variety of biological aerosol particles found in the atmosphere are the pictured brochosomes, which are released by insects. Atmospheric chemistry and physics, the biosphere, the hydrological cycle, climate, and human health are all strongly influenced by natural and anthropogenic particles in the nanometer to micrometer size range.
Atmospheric aerosols and fine particulate matter (PM
) are strongly affecting human health and climate in the Anthropocene, that is, in the current era of globally pervasive and rapidly increasing ...human influence on planet Earth. Poor air quality associated with high aerosol concentrations is among the leading health risks worldwide, causing millions of attributable excess deaths and years of life lost every year. Besides their health impact, aerosols are also influencing climate through interactions with clouds and solar radiation with an estimated negative total effective radiative forcing that may compensate about half of the positive radiative forcing of carbon dioxide but exhibits a much larger uncertainty. Heterogeneous and multiphase chemical reactions on the surface and in the bulk of solid, semisolid, and liquid aerosol particles have been recognized to influence aerosol formation and transformation and thus their environmental effects. However, atmospheric multiphase chemistry is not well understood because of its intrinsic complexity of dealing with the matter in multiple phases and the difficulties of distinguishing its effect from that of gas phase reactions.Recently, research on atmospheric multiphase chemistry received a boost from the growing interest in understanding severe haze formation of very high PM
concentrations in polluted megacities and densely populated regions. State-of-the-art models suggest that the gas phase reactions, however, are not capturing the high concentrations and rapid increase of PM
observed during haze events, suggesting a gap in our understanding of the chemical mechanisms of aerosol formation. These haze events are characterized by high concentrations of aerosol particles and high humidity, especially favoring multiphase chemistry. In this Account, we review recent advances that we have made, as well as current challenges and future perspectives for research on multiphase chemical processes involved in atmospheric aerosol formation and transformation. We focus on the following questions: what are the key reaction pathways leading to aerosol formation under polluted conditions, what is the relative importance of multiphase chemistry versus gas-phase chemistry, and what are the implications for the development of efficient and reliable air quality control strategies? In particular, we discuss advances and challenges related to different chemical regimes of sulfate, nitrate, and secondary organic aerosols (SOAs) under haze conditions, and we synthesize new insights into the influence of aerosol water content, aerosol pH, phase state, and nanoparticle size effects. Overall, there is increasing evidence that multiphase chemistry plays an important role in aerosol formation during haze events. In contrast to the gas phase photochemical reactions, which are self-buffered against heavy pollution, multiphase reactions have a positive feedback mechanism, where higher particle matter levels accelerate multiphase production, which further increases the aerosol concentration resulting in a series of record-breaking pollution events. We discuss perspectives to fill the gap of the current understanding of atmospheric multiphase reactions that involve multiple physical and chemical processes from bulk to nanoscale and from regional to global scales. A synthetic approach combining laboratory experiments, field measurements, instrument development, and model simulations is suggested as a roadmap to advance future research.
Recently, it has been proposed that organic aerosol particles in the atmosphere can exist in an amorphous semi-solid or solid (i.e. glassy) state. In this perspective, we analyse and discuss the ...formation and properties of amorphous semi-solids and glasses from organic liquids. Based on a systematic survey of a wide range of organic compounds, we present estimates for the glass forming properties of atmospheric secondary organic aerosol (SOA). In particular we investigate the dependence of the glass transition temperature T(g) upon various molecular properties such as the compounds' melting temperature, their molar mass, and their atomic oxygen-to-carbon ratios (O:C ratios). Also the effects of mixing different compounds and the effects of hygroscopic water uptake depending on ambient relative humidity are investigated. In addition to the effects of temperature, we suggest that molar mass and water content are much more important than the O:C ratio for characterizing whether an organic aerosol particle is in a liquid, semi-solid, or glassy state. Moreover, we show how the viscosity in liquid, semi-solid and glassy states affect the diffusivity of those molecules constituting the organic matrix as well as that of guest molecules such as water or oxidants, and we discuss the implications for atmospheric multi-phase processes. Finally, we assess the current state of knowledge and the level of scientific understanding, and we propose avenues for future studies to resolve existing uncertainties.
Abstract
Aims
Ambient air pollution is a major health risk, leading to respiratory and cardiovascular mortality. A recent Global Exposure Mortality Model, based on an unmatched number of cohort ...studies in many countries, provides new hazard ratio functions, calling for re-evaluation of the disease burden. Accordingly, we estimated excess cardiovascular mortality attributed to air pollution in Europe.
Methods and results
The new hazard ratio functions have been combined with ambient air pollution exposure data to estimate the impacts in Europe and the 28 countries of the European Union (EU-28). The annual excess mortality rate from ambient air pollution in Europe is 790 000 95% confidence interval (95% CI) 645 000–934 000, and 659 000 (95% CI 537 000–775 000) in the EU-28. Between 40% and 80% are due to cardiovascular events, which dominate health outcomes. The upper limit includes events attributed to other non-communicable diseases, which are currently not specified. These estimates exceed recent analyses, such as the Global Burden of Disease for 2015, by more than a factor of two. We estimate that air pollution reduces the mean life expectancy in Europe by about 2.2 years with an annual, attributable per capita mortality rate in Europe of 133/100 000 per year.
Conclusion
We provide new data based on novel hazard ratio functions suggesting that the health impacts attributable to ambient air pollution in Europe are substantially higher than previously assumed, though subject to considerable uncertainty. Our results imply that replacing fossil fuels by clean, renewable energy sources could substantially reduce the loss of life expectancy from air pollution.
Water content and mass matter more than composition for the acidity of atmospheric aerosols in ammonia-buffered regions.
A multiphasic effect
Aerosols exert a primary influence on atmospheric ...chemistry. One of the main controls on their internal chemistry is their acidity, so understanding what determines aerosol pH is fundamental for determining their environmental effects. Zheng
et al.
considered how buffering capacity in a multiphase aerosol system differs from bulk solution and found an important role for water content in determining pH in ammonia-buffered regions. Their conclusions underscore the important influence of ammonia emissions in the Anthropocene.
Science
, this issue p.
1374
Aerosol acidity largely regulates the chemistry of atmospheric particles, and resolving the drivers of aerosol pH is key to understanding their environmental effects. We find that an individual buffering agent can adopt different buffer pH values in aerosols and that aerosol pH levels in populated continental regions are widely buffered by the conjugate acid-base pair NH
4
+
/NH
3
(ammonium/ammonia). We propose a multiphase buffer theory to explain these large shifts of buffer pH, and we show that aerosol water content and mass concentration play a more important role in determining aerosol pH in ammonia-buffered regions than variations in particle chemical composition. Our results imply that aerosol pH and atmospheric multiphase chemistry are strongly affected by the pervasive human influence on ammonia emissions and the nitrogen cycle in the Anthropocene.
The formation and aging of organic aerosols (OA) proceed through multiple steps of chemical reaction and mass transport in the gas and particle phases, which is challenging for the interpretation of ...field measurements and laboratory experiments as well as accurate representation of OA evolution in atmospheric aerosol models. Based on data from over 30 000 compounds, we show that organic compounds with a wide variety of functional groups fall into molecular corridors, characterized by a tight inverse correlation between molar mass and volatility. We developed parameterizations to predict the saturation mass concentration of organic compounds containing oxygen, nitrogen, and sulfur from the elemental composition that can be measured by soft-ionization high-resolution mass spectrometry. Field measurement data from new particle formation events, biomass burning, cloud/fog processing, and indoor environments were mapped into molecular corridors to characterize the chemical nature of the observed OA components. We found that less-oxidized indoor OA are constrained to a corridor of low molar mass and high volatility, whereas highly oxygenated compounds in atmospheric water extend to high molar mass and low volatility. Among the nitrogen- and sulfur-containing compounds identified in atmospheric aerosols, amines tend to exhibit low molar mass and high volatility, whereas organonitrates and organosulfates follow high O : C corridors extending to high molar mass and low volatility. We suggest that the consideration of molar mass and molecular corridors can help to constrain volatility and particle-phase state in the modeling of OA particularly for nitrogen- and sulfur-containing compounds.
Air pollution contributes to the premature deaths of millions of people each year around the world, and air quality problems are growing in many developing nations. While past policy efforts have ...succeeded in reducing particulate matter and trace gases in North America and Europe, adverse health effects are found at even these lower levels of air pollution. Future policy actions will benefit from improved understanding of the interactions and health effects of different chemical species and source categories. Achieving this new understanding requires air pollution scientists and engineers to work increasingly closely with health scientists. In particular, research is needed to better understand the chemical and physical properties of complex air pollutant mixtures, and to use new observations provided by satellites, advanced in situ measurement techniques, and distributed micro monitoring networks, coupled with models, to better characterize air pollution exposure for epidemiological and toxicological research, and to better quantify the effects of specific source sectors and mitigation strategies.
Poor air quality is globally the largest environmental health risk. Epidemiological studies have uncovered clear relationships of gaseous pollutants and particulate matter (PM) with adverse health ...outcomes, including mortality by cardiovascular and respiratory diseases. Studies of health impacts by aerosols are highly multidisciplinary with a broad range of scales in space and time. We assess recent advances and future challenges regarding aerosol effects on health from molecular to global scales through epidemiological studies, field measurements, health-related properties of PM, and multiphase interactions of oxidants and PM upon respiratory deposition. Global modeling combined with epidemiological exposure-response functions indicates that ambient air pollution causes more than four million premature deaths per year. Epidemiological studies usually refer to PM mass concentrations, but some health effects may relate to specific constituents such as bioaerosols, polycyclic aromatic compounds, and transition metals. Various analytical techniques and cellular and molecular assays are applied to assess the redox activity of PM and the formation of reactive oxygen species. Multiphase chemical interactions of lung antioxidants with atmospheric pollutants are crucial to the mechanistic and molecular understanding of oxidative stress upon respiratory deposition. The role of distinct PM components in health impacts and mortality needs to be clarified by integrated research on various spatiotemporal scales for better evaluation and mitigation of aerosol effects on public health in the Anthropocene.
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