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      Rapid mass growth and enhanced light extinction of atmospheric aerosols during the heating season haze episodes in Beijing revealed by aerosol–chemistry–radiation–boundary layer interaction

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          Abstract

          Abstract. Despite the numerous studies investigating haze formation mechanism in China, it is still puzzling that intensive haze episodes could form within hours directly following relatively clean periods. Haze has been suggested to be initiated by the variation of meteorological parameters and then to be substantially enhanced by aerosol–radiation–boundary layer feedback. However, knowledge on the detailed chemical processes and the driving factors for extensive aerosol mass accumulation during the feedback is still scarce. Here, the dependency of the aerosol number size distribution, mass concentration and chemical composition on the daytime mixing layer height (MLH) in urban Beijing is investigated. The size distribution and chemical composition-resolved dry aerosol light extinction is also explored. The results indicate that the aerosol mass concentration and fraction of nitrate increased dramatically when the MLH decreased from high to low conditions, corresponding to relatively clean and polluted conditions, respectively. Particles having their dry diameters in the size of ∼400–700 nm, and especially particle-phase ammonium nitrate and liquid water, contributed greatly to visibility degradation during the winter haze periods. The dependency of aerosol composition on the MLH revealed that ammonium nitrate and aerosol water content increased the most during low MLH conditions, which may have further triggered enhanced formation of sulfate and organic aerosol via heterogeneous reactions. As a result, more sulfate, nitrate and water-soluble organics were formed, leading to an enhanced water uptake ability and increased light extinction by the aerosols. The results of this study contribute towards a more detailed understanding of the aerosol–chemistry–radiation–boundary layer feedback that is likely to be responsible for explosive aerosol mass growth events in urban Beijing.

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          Most cited references51

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          The contribution of outdoor air pollution sources to premature mortality on a global scale.

          Assessment of the global burden of disease is based on epidemiological cohort studies that connect premature mortality to a wide range of causes, including the long-term health impacts of ozone and fine particulate matter with a diameter smaller than 2.5 micrometres (PM2.5). It has proved difficult to quantify premature mortality related to air pollution, notably in regions where air quality is not monitored, and also because the toxicity of particles from various sources may vary. Here we use a global atmospheric chemistry model to investigate the link between premature mortality and seven emission source categories in urban and rural environments. In accord with the global burden of disease for 2010 (ref. 5), we calculate that outdoor air pollution, mostly by PM2.5, leads to 3.3 (95 per cent confidence interval 1.61-4.81) million premature deaths per year worldwide, predominantly in Asia. We primarily assume that all particles are equally toxic, but also include a sensitivity study that accounts for differential toxicity. We find that emissions from residential energy use such as heating and cooking, prevalent in India and China, have the largest impact on premature mortality globally, being even more dominant if carbonaceous particles are assumed to be most toxic. Whereas in much of the USA and in a few other countries emissions from traffic and power generation are important, in eastern USA, Europe, Russia and East Asia agricultural emissions make the largest relative contribution to PM2.5, with the estimate of overall health impact depending on assumptions regarding particle toxicity. Model projections based on a business-as-usual emission scenario indicate that the contribution of outdoor air pollution to premature mortality could double by 2050.
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            Evolution of organic aerosols in the atmosphere.

            Organic aerosol (OA) particles affect climate forcing and human health, but their sources and evolution remain poorly characterized. We present a unifying model framework describing the atmospheric evolution of OA that is constrained by high-time-resolution measurements of its composition, volatility, and oxidation state. OA and OA precursor gases evolve by becoming increasingly oxidized, less volatile, and more hygroscopic, leading to the formation of oxygenated organic aerosol (OOA), with concentrations comparable to those of sulfate aerosol throughout the Northern Hemisphere. Our model framework captures the dynamic aging behavior observed in both the atmosphere and laboratory: It can serve as a basis for improving parameterizations in regional and global models.
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              Trends in China's anthropogenic emissions since 2010 as the consequence of clean air actions

              Abstract. To tackle the problem of severe air pollution, China has implemented active clean air policies in recent years. As a consequence, the emissions of major air pollutants have decreased and the air quality has substantially improved. Here, we quantified China's anthropogenic emission trends from 2010 to 2017 and identified the major driving forces of these trends by using a combination of bottom-up emission inventory and index decomposition analysis (IDA) approaches. The relative change rates of China's anthropogenic emissions during 2010–2017 are estimated as follows: −62 % for SO 2 , −17 % for NO x , +11 % for nonmethane volatile organic compounds (NMVOCs), +1 % for NH 3 , −27 % for CO, −38 % for PM 10 , −35 % for PM 2.5 , −27 % for BC, −35 % for OC, and +16 % for CO 2 . The IDA results suggest that emission control measures are the main drivers of this reduction, in which the pollution controls on power plants and industries are the most effective mitigation measures. The emission reduction rates markedly accelerated after the year 2013, confirming the effectiveness of China's Clean Air Action that was implemented since 2013. We estimated that during 2013–2017, China's anthropogenic emissions decreased by 59 % for SO 2 , 21 % for NO x , 23 % for CO, 36 % for PM 10 , 33 % for PM 2.5 , 28 % for BC, and 32 % for OC. NMVOC emissions increased and NH 3 emissions remained stable during 2010–2017, representing the absence of effective mitigation measures for NMVOCs and NH 3 in current policies. The relative contributions of different sectors to emissions have significantly changed after several years' implementation of clean air policies, indicating that it is paramount to introduce new policies to enable further emission reductions in the future.
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                Author and article information

                Contributors
                Journal
                Atmospheric Chemistry and Physics
                Atmos. Chem. Phys.
                Copernicus GmbH
                1680-7324
                2021
                August 16 2021
                : 21
                : 16
                : 12173-12187
                Article
                10.5194/acp-21-12173-2021
                fb532a92-7616-4bde-8a1f-46484910998b
                © 2021

                https://creativecommons.org/licenses/by/4.0/

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