Changes In Aerosol Composition Research Articles

A Regional Aerosol Model for the Oceanic Area around Eastern China Based on Aerosol Robotic Network (AERONET)

A regional aerosol model can complement globally averaged models and improve the accuracy of atmospheric numerical models in local applications. This study established a seasonal aerosol model based on data from the Aerosol Robotic Network (AERONET) of the sea area around eastern China, and its performance in calculating the aerosol optical depth (AOD) was evaluated. The seasonal columnar volume particle size distributions (VPSDs) illustrated a bimodal structure consisting of fine and coarse modes. The VPSDs of spring, autumn, and winter roughly agreed with each other, with their amplitudes of fine and coarse modes being almost equal; however, the fine mode of the summer VPSD was approximately twice as high as that of the coarse mode. Lognormal mode decomposition analysis revealed that fine and coarse modes comprised two sub-modes. Fitting the seasonal VPSDs to the four-mode lognormal distribution yielded a parameterized aerosol size distribution model. Furthermore, seasonal variations in complex refractive indices (CRIs) indicated unignorable changes in aerosol compositions. Overall, error analysis validated that the proposed model could meet accuracy requirements for optical engineering applications, with median AOD calculation errors of less than 0.01.

Significant Reductions in Secondary Aerosols after the Three-Year Action Plan in Beijing Summer.

Air quality in China has continuously improved during the Three-Year Action Plan (2018-2020); however, the changes in aerosol composition, properties, and sources in Beijing summer remain poorly understood. Here, we conducted real-time measurements of aerosol composition in five summers from 2018 to 2022 along with WRF-Community Multiscale Air Quality simulations to characterize the changes in aerosol chemistry and the roles of meteorology and emission reductions. Largely different from winter, secondary inorganic aerosol and photochemical-related secondary organic aerosol (SOA) showed significant decreases by 55-67% in summer, and the most decreases occurred in 2021. Comparatively, the decreases in the primary aerosol species and gaseous precursors were comparably small. While decreased atmospheric oxidation capacity as indicated by ozone changes played an important role in changing SOA composition, the large decrease in aerosol liquid water and small increase in particle acidity were critical for nitrate changes by decreasing gas-particle partitioning substantially (∼28%). Analysis of meteorological influences demonstrated clear and similar transitions in aerosol composition and formation mechanisms at a relative humidity of 50-60% in five summers. Model simulations revealed that emission controls played the decisive role in reducing sulfate, primary OA, and anthropogenic SOA during the Three-Year Action Plan, while meteorology affected more nitrate and biogenic SOA.

Atmospheric mercury in a developed region of eastern China: Interannual variation and gas-particle partitioning

Atmospheric mercury plays a crucial role in the biogeochemical cycle of mercury. This study conducted an intensive measurement of atmospheric mercury from 2015 to 2018 at a regional site in eastern China. During this period, the concentration of particle-bound mercury (PBM) decreased by 13%, which was much lower than those of gaseous elemenral mercury (GEM, 30%) and reactive gaseous mercury (GOM, 62%). The gradual decrease in the correlation between PBM and CO, K, and Pb indicates that the influence of primary emissions on PBM concentration was weakening. Moreover, the value of the partitioning coefficient (Kp) increased gradually from 0.05 ± 0.076 m3/μg in 2015 to 0.16 ± 0.37 m3/μg in 2018, indicating that GOM was increasingly inclined to adsorb onto particulate matter. Excluding the influence of meteorological conditions and the primary emissions, the change in aerosol composition is designated as the main trigger factor for the increasing gas-particle partitioning of reactive mercury (RM). The increasing ratio of Cl−, NO3−, and organics (Org) in the chemical composition of particle matters (PM2.5), as well as the decrease in the proportion of SO42−, NH4+, and K+, are conducive to the adsorption of GOM onto particles, forming PBM, which led to an increase of Kp and a lag of PBM reduction compared to GEM and GOM under the continuous control measures of anthropogenic mercury emissions. The evolution of aerosol compositions in recent years affects the migration and transformation of atmospheric mercury, which in turn can affect the biogeochemical cycle of mercury.

Impact of shipping emissions regulation on urban aerosol composition changes revealed by receptor and numerical modelling

Various shipping emissions controls have recently been implemented at both local and national scales. However, it is difficult to track the effect of these on PM2.5 levels, owing to the non-linear relationship that exists between changes in precursor emissions and PM components. Positive Matrix Factorisation (PMF) identifies that a switch to cleaner fuels since January 2020 results in considerable reductions in shipping-source-related PM2.5, especially sulphate aerosols and metals (V and Ni), not only at a port site but also at an urban background site. CMAQ sensitivity analysis reveals that the reduction of secondary inorganic aerosols (SIA) further extends to inland areas downwind from ports. In addition, mitigation of secondary organic aerosols (SOA) in coastal urban areas can be anticipated either from the results of receptor modelling or from CMAQ simulations. The results in this study show the possibility of obtaining human health benefits in coastal cities through shipping emission controls.

Changes in primary and secondary aerosols during a controlled Chinese New Year

Large reductions in anthropogenic emissions during the Chinese New Year (CNY) holiday in Beijing have been well reported. However, the changes during the CNY of 2021 are different because most people stayed in Beijing to control the spread of coronavirus disease (COVID-19). Here a high-resolution aerosol mass spectrometer (HR-AMS) was deployed for characterization of the changes in size-resolved aerosol composition and sources during the CNY. We found that the reductions in traffic-related NOx and fossil fuel-related organic aerosol (OA), and cooking OA (1.3–12.7%) during the CNY of 2021 were much smaller than those in previous CNY holidays of 2013, 2015, and 2020. In contrast, the mass concentrations of secondary aerosol species except nitrate showed ubiquitous increases (17.6–30.4%) during the CNY of 2021 mainly due to a 4-day severe haze episode. OA composition also changed substantially during the CNY of 2021. In particular, we observed a large increase by nearly a factor of 2 in oxidized primary OA likely from biomass burning, and a decrease of 50.1% in aqueous-phase secondary OA. A further analysis of the severe haze episode during the CNY illustrated a rapid transition of secondary formation from photochemical to aqueous-phase processing followed by a scavenging process, leading to significant changes in aerosol composition, size distributions, and oxidation degree of OA. A parameterization relationship between oxygen-to-carbon (O/C) and f44 (fraction of m/z 44 in OA) from a collocated capture vaporizer aerosol chemical speciation monitor (CV-ACSM) was developed, which has a significant implication for characterization of OA evolution and the impacts on hygroscopicity due to the rapidly increased deployments of CV-ACSM worldwide.

Clear-sky spectral radiance modeling under variable aerosol conditions

The distribution of diffuse radiance over the sky hemisphere is an important quantity that is required in many applications. Its spectral variation is useful when considering processes having a spectral dependence, such as photovoltaics (PV). Here, a clear-sky spectral radiance model is developed from radiative transfer theory, using appropriate parameterizations to make the model suitable for rapid engineering-type calculations. The phase function of various aerosol mixtures combines three conventional Henyey-Greenstein functions. This procedure provides an effective solution to the problem of modeling the strong radiance within the circumsolar region, while being also accurate in low-energy areas of the clear sky. The dependence on wavelength of the coefficients of the simplified phase functions is efficiently described by polynomial ratios. The radiance is shown to vary from a relatively isotropic distribution in the UV to a very anisotropic one over the rest of the solar spectrum. The radiance model can be used to describe either ideal atmospheric situations or dynamic situations, for which the hourly outputs from the MERRA-2 reanalysis provide the optical properties of the aerosol mixture at any location. Examples of ideal radiance distributions include those corresponding to the reference spectra used for the performance characterization of PV cells. By integrating the modeled radiance over all wavelengths with appropriate weighting, both the broadband radiance and luminance can be derived. Although these two distributions are generally not identical, they are found sufficiently close, even under hazy conditions, to make them interchangeable in practice, within reasonable error limits. Compared to common empirical luminance distributions of the literature, the model appears more universal, because responsive to strong changes in aerosol composition.

Dramatic changes in aerosol composition during the 2016–2020 heating seasons in Beijing–Tianjin–Hebei region and its surrounding areas: The role of primary pollutants and secondary aerosol formation

With the implementation of a series of air pollution mitigation strategies during the past decade, great air quality improvements have been observed in the BTH region. Despite of significant decreases in gaseous pollutants, such as SO2 and NO2, the enhancement of secondary aerosol formation was observed. NO3− has surpassed SO42− and OM to become the dominant PM2.5 component. We find that the reduction of POC mainly dominated the decreasing trend of OC. As for secondary inorganic components, the key processes or factors controlling the spatial-temporal variation characteristics were different. The areas with large SO42− concentrations corresponded well to those with high SO2 concentrations, while the synchronized NO3− better followed spatial patterns in O3 than NO2. From 2016 to 2020, the response of SO42− to SO2 was close to a linear function, while the reaction of NO3− to the decrease of NO2 displayed nonlinear behavior. Such different relationships indicated that SO42− was predominantly controlled by SO2, while NO3− was not only related to NO2 but also determined by the secondary conversion process. The ratios of SO42−, NO3−, NH4+, and OC to EC between 2016 and 2020 were generally higher than 1 in typical BTH cities, and the ratio of NO3− to EC was exceptionally high, with a range reaching up to 200 %. Besides, this ratio coincided well with the enhancement of Ox, indicating the potential role of Ox to secondary NO3− formation. The diurnal cycle of NO3−, O3, and NO2 concentration change rate indicated that the relative increase of O3 during nighttime may offset the effectiveness of NOX emission reduction. This study provided observational evidence of enhanced secondary NO3− formation with the rising trend of atmospheric oxidation and emphasized the importance of nighttime chemistry for NO3− formation in the BTH region.

Aerosols from anthropogenic and biogenic sources and their interactions – modeling aerosol formation, optical properties, and impacts over the central Amazon basin

Abstract. The Green Ocean Amazon experiment – GoAmazon 2014–2015 – explored the interactions between natural biogenic forest emissions from central Amazonia and urban air pollution from Manaus. Previous GoAmazon 2014–2015 studies showed that nitrogen oxide (NOx = NO + NO2) and sulfur oxide (SOx) emissions from Manaus strongly interact with biogenic volatile organic compounds (BVOCs), affecting secondary organic aerosol (SOA) formation. In previous studies, ground-based and aircraft measurements provided evidence of SOA formation and strong changes in aerosol composition and properties. Aerosol optical properties also evolve, and their impacts on the Amazonian ecosystem can be significant. As particles age, some processes, such as SOA production, black carbon (BC) deposition, particle growth and the BC lensing effect change the aerosol optical properties, affecting the solar radiation flux at the surface. This study analyzes data and models SOA formation using the Weather Research and Forecasting with Chemistry (WRF-Chem) model to assess the spatial variability in aerosol optical properties as the Manaus plumes interact with the natural atmosphere. The following aerosol optical properties are investigated: single scattering albedo (SSA), asymmetry parameter (gaer), absorption Ångström exponent (AAE) and scattering Ångström exponent (SAE). These simulations were validated using ground-based measurements at three experimental sites, namely the Amazon Tall Tower Observatory – ATTO (T0a), downtown Manaus (T1), Tiwa Hotel (T2) and Manacapuru (T3), as well as the U.S. Department of Energy (DOE) Gulfstream 1 (G-1) aircraft flights. WRF-Chem simulations were performed over 7 d during March 2014. Results show a mean biogenic SOA (BSOA) mass enrichment of 512 % at the T1 site, 450 % in regions downwind of Manaus, such as the T3 site, and 850 % in areas north of the T3 site in simulations with anthropogenic emissions. The SOA formation is rather fast, with about 80 % of the SOA mass produced in 3–4 h. Comparing the plume from simulations with and without anthropogenic emissions, SSA shows a downwind reduction of approximately 10 %, 11 % and 6 % at the T1, T2 and T3 sites, respectively. Other regions, such as those further downwind of the T3 site, are also affected. The gaer values increased from 0.62 to 0.74 at the T1 site and from 0.67 to 0.72 at the T3 site when anthropogenic emissions are active. During the Manaus plume-aging process, a plume tracking analysis shows an increase in SSA from 0.91 close to Manaus to 0.98 160 km downwind of Manaus as a result of SOA production and BC deposition.

Changes in Aerosol Composition over East Asia Due to the Emission Regulations in China

Changes in Aerosol Composition over East Asia Due to the Emission Regulations in China

Simulation of Atmospheric Visibility Impairment.

Changes in aerosol composition and its proportions can cause changes in atmospheric visibility. Vision systems deployed outdoors must take into account the negative effects brought by visibility impairment. In order to develop vision algorithms that can adapt to low atmospheric visibility conditions, a large-scale dataset containing pairs of clear images and their visibility-impaired versions (along with other annotations if necessary) is usually indispensable. However, it is almost impossible to collect large amounts of such image pairs in a real physical environment. A natural and reasonable solution is to use virtual simulation technologies, which is also the focus of this paper. In this paper, we first deeply analyze the limitations and irrationalities of the existing work specializing on simulation of atmospheric visibility impairment. We point out that many simulation schemes actually even violate the assumptions of the Koschmieder's law. Second, more importantly, based on a thorough investigation of the relevant studies in the field of atmospheric science, we present simulation strategies for five most commonly encountered visibility impairment phenomena, including mist, fog, natural haze, smog, and Asian dust. Our work establishes a direct link between the fields of atmospheric science and computer vision. In addition, as a byproduct, with the proposed simulation schemes, a large-scale synthetic dataset is established, comprising 40,000 clear source images and their 800,000 visibility-impaired versions. To make our work reproducible, source codes and the dataset have been released at https://cslinzhang.github.io/AVID/.

Significant changes in autumn and winter aerosol composition and sources in Beijing from 2012 to 2018: Effects of clean air actions.

A seven-year long-term comprehensive measurement of non-refractory submicron particles (NR-PM1) in autumn and winter in Beijing from 2012 to 2018 was conducted to evaluate the effectiveness of the clean air actions implemented by the Chinese government in September 2013 on aerosols from different sources and chemical processes. Results showed that the NR-PM1 concentrations decreased by 44.1% in autumn and 73.2% in winter from 2012 to 2018. Sulfate showed a much larger reduction than nitrate and ammonium in both autumn (55%) and winter (86%) and that nitrate even slightly increased by 15.8% in autumn. As a result, aerosol pollution in winter gradually changed from sulfate-rich to nitrate-rich with a sudden change after 2016 and the dominant role of nitrate in autumn was also strengthened after 2016. Among primary organic aerosol (OA) types, biomass burning OA and coal combustion OA exhibited the largest decline in autumn and winter, with reductions of 87.5% and 77.3%, respectively, while hydrocarbon-like OA (HOA) exhibited the smallest decline in both autumn (24.4%) and winter (37.1%). These significant changes in aerosol compositions were highly consistent with the much faster reduction of SO2 (75-85%) than NOx (36-59%) and were mainly due to the clean air actions rather than the impact of meteorological conditions. What's more, the enhanced atmospheric oxidizing capacity, which was indicated by increased O3, altered the chemical processes of oxygenated OA (OOA), especially in autumn. Both of less-oxidized OOA (LO-OOA) and more-oxidized OOA showed elevated contributions in OA by 4% in autumn. The increased oxygen-to-carbon ratios of LO-OOA in autumn (from 0.42 to 0.58) and winter (from 0.44 to 0.52) indicated the enhanced atmospheric oxidizing capacity strengthened photochemical reactions and resulted in the increased oxidation degree of LO-OOA. This study demonstrates the effectiveness of the clean air actions for air quality improvement in Beijing.

An experimental investigation into the operation of an electrically heated tobacco system

An experimental investigation of the thermal processes taking place in the tobacco substrate of a recently developed multicomponent electrically heated tobacco product (EHTP) that is part of an electrically heated tobacco system (EHTS – also referred to as the Tobacco Heating System 2.2) was carried out. Temperature profiles in the tobacco substrate of the EHTP were characterized using thermocouples positioned at different distances from the heater surface. The average maximum temperature of the tobacco measured 0.2 mm from the heater’s surface was < 260 °C, well below the temperature required for the self-sustaining smoldering combustion of the tobacco substrate to occur. The chemical composition of the aerosol generated from the EHTP when the EHTS was operated under oxidative and non-oxidative atmospheres was investigated. The aerosol derived from the controlled heating of the tobacco substrate is comprised principally of water, nicotine and glycerol that are evaporated from the tobacco substrate. No significant change in aerosol composition and in the amounts of CO, NO and NOx were detected when comparing the aerosol formed under non-oxidative (where combustion processes cannot occur) and oxidative atmospheres.

Response of aerosol chemistry to clean air action in Beijing, China: Insights from two-year ACSM measurements and model simulations

Despite substantial mitigation of particulate matter (PM) pollution during the past decade in Beijing, the response of aerosol chemistry to clean air action and meteorology remains less understood. Here we characterized the changes in aerosol composition as responses to emission reductions by using two-year long-term measurements in 2011/2012 and 2017/2018, and WRF-Chem model. Our results showed substantial decreases for all aerosol species except nitrate from 2011/2012 to 2017/2018. Chloride exhibited the largest decrease by 65–89% followed by organics (37–70%), mainly due to reductions in coal combustion emissions in winter and agriculture burning in June. Primary and secondary organic aerosol (SOA) showed comparable decreases by 61–70% in fall and winter, and 34–63% in spring and summer, suggesting that reductions in primary emissions might also suppress SOA formation. The changes in nitrate were negligible and even showed increases due to less reductions in NOx emissions and increased formation potential from N2O5 heterogeneous reactions. As a result, nitrate exceeded sulfate and became the major secondary inorganic aerosol species in PM with the contribution increasing from 14–21% to 22–32%. Further analysis indicated that the reductions in aerosol species from 2011/2012 to 2017/2018 were mainly caused by the decreases of severely polluted events (PM1 > 100 μg m−3). WRF-Chem simulations suggested that the decreases in OA and sulfate in fall and winter were mainly resulted from emission reductions (27–36% and 25–43%) and favorable meteorology (4–10% and 19–30%), while they were dominantly contributed by emission changes in spring and summer. Comparatively, the changes in nitrate were mainly associated with meteorological variations while the contributions of emissions changes were relatively small. Our results highlight different chemical responses of aerosol species to emission changes and meteorology, suggesting that future mitigation of air pollution in China needs species-targeted control policy.

Rapid transition in winter aerosol composition in Beijing from 2014 to 2017: response to clean air actions

Abstract. The clean air actions implemented by the Chinese government in 2013 have led to significantly improved air quality in Beijing. In this work, we combined the in situ measurements of the chemical components of submicron particles (PM1) in Beijing during the winters of 2014 and 2017 and a regional chemical transport model to investigate the impact of clean air actions on aerosol chemistry and quantify the relative contributions of anthropogenic emissions, meteorological conditions, and regional transport to the changes in aerosol chemical composition from 2014 to 2017. We found that the average PM1 concentration in winter in Beijing decreased by 49.5 % from 2014 to 2017 (from 66.2 to 33.4 µg m−3). Sulfate exhibited a much larger decline than nitrate and ammonium, which led to a rapid transition from sulfate-driven to nitrate-driven aerosol pollution during the wintertime. Organic aerosol (OA), especially coal combustion OA, and black carbon also showed large decreasing rates, indicating the effective emission control of coal combustion and biomass burning. The decreased sulfate contribution and increased nitrate fraction were highly consistent with the much faster emission reductions in sulfur dioxide (SO2) due to phasing out coal in Beijing compared to reduction in nitrogen oxides emissions estimated by bottom-up inventory. The chemical transport model simulations with these emission estimates reproduced the relative changes in aerosol composition and suggested that the reduced emissions in Beijing and its surrounding regions played a dominant role. The variations in meteorological conditions and regional transport contributed much less to the changes in aerosol concentration and its chemical composition during 2014–2017 compared to the decreasing emissions. Finally, we speculated that changes in precursor emissions possibly altered the aerosol formation mechanisms based on ambient observations. The observed explosive growth of sulfate at a relative humidity (RH) greater than 50 % in 2014 was delayed to a higher RH of 70 % in 2017, which was likely caused by the suppressed sulfate formation through heterogeneous reactions due to the decrease in SO2 emissions. Thermodynamic simulations showed that the decreased sulfate and nitrate concentrations have lowered the aerosol water content, particle acidity, and ammonium particle fraction. The results in this study demonstrate the response of aerosol chemistry to the stringent clean air actions and identify that the anthropogenic emission reductions are a major driver, which could help to further guide air pollution control strategies in China.

Compositional evolution of particle-phase reaction products and water in the heterogeneous OH oxidation of model aqueous organic aerosols

Abstract. Organic compounds present at or near the surface of aqueous droplets can be efficiently oxidized by gas-phase OH radicals, which alter the molecular distribution of the reaction products within the droplet. A change in aerosol composition affects the hygroscopicity and leads to a concomitant response in the equilibrium amount of particle-phase water. The variation in the aerosol water content affects the aerosol size and physicochemical properties, which in turn governs the oxidation kinetics and chemistry. To attain better knowledge of the compositional evolution of aqueous organic droplets during oxidation, this work investigates the heterogeneous OH-radical-initiated oxidation of aqueous methylsuccinic acid (C5H8O4) droplets, a model compound for small branched dicarboxylic acids found in atmospheric aerosols, at a high relative humidity of 85 % through experimental and modeling approaches. Aerosol mass spectra measured by a soft atmospheric pressure ionization source (Direct Analysis in Real Time, DART) coupled with a high-resolution mass spectrometer reveal two major products: a five carbon atom (C5) hydroxyl functionalization product (C5H8O5) and a C4 fragmentation product (C4H6O3). These two products likely originate from the formation and subsequent reactions (intermolecular hydrogen abstraction and carbon–carbon bond scission) of tertiary alkoxy radicals resulting from the OH abstraction occurring at the methyl-substituted carbon site. Based on the identification of the reaction products, a kinetic model of oxidation (a two-product model) coupled with the Aerosol Inorganic–Organic Mixtures Functional groups Activity Coefficients (AIOMFAC) model is built to simulate the size and compositional changes of aqueous methylsuccinic acid droplets during oxidation. Model results show that at the maximum OH exposure, the droplets become slightly more hygroscopic after oxidation, as the mass fraction of water is predicted to increase from 0.362 to 0.424; however, the diameter of the droplets decreases by 6.1 %. This can be attributed to the formation of volatile fragmentation products that partition to the gas phase, leading to a net loss of organic species and associated particle-phase water, and thus a smaller droplet size. Overall, fragmentation and volatilization processes play a larger role than the functionalization process in determining the evolution of aerosol water content and droplet size at high-oxidation stages.

The influence of continental air masses on the aerosols and nutrients deposition over the western North Pacific

The air masses transported from East Asia have a strong impact on the aerosol properties and deposition in the marine boundary layer of the western North Pacific (WNP) during winter and spring. We joined a cruise between 17 Mar. and 22 Apr. 2014 and investigated the changes of aerosol composition and size distribution over the remote WNP and marginal seas. Although the secondary aerosol species (SO42−, NO3− and NH4+) in remote WNP were influenced significantly by the continental transport, NH4+ concentrations were lower than 2.7 μg m−3 in most sampling days and not correlated with non-sea-salt (nss)-SO42- suggesting that the ocean could be a primary source of NH4+. Moderate Cl− depletion (23%) was observed in remote WNP, and the inverse relationship between Cl− depletion percentages and nss-K+ in aerosols suggested that the transport of biomass burning smoke from East Asia might be a vital extra source of Cl−. Both Asian dust and haze events were encountered during the cruise. Asian dust carried large amounts of crustal elements such as Al and Ti to the WNP, and the dusty Fe deposition may double its background concentration in seawater. Differently, a dramatic increase of dry deposition flux of dissolved particulate inorganic nitrogen was observed during the haze event. Our study reveals that the transport of different continental air masses may have distinct biogeochemical impacts on the WNP by increasing the fluxes of different nutrient elements and potentially changing the nutrient stoichiometry.

CCN characteristics over a tropical coastal station during south-west monsoon: observations and closure studies

Number concentration measurements of cloud condensation nuclei (CCN) at five supersaturation values between 0.2 and 1.0% were made from a coastal site (Thiruvananthapuram) of peninsular India using a single column CCN counter during the summer monsoon period (June–September) of 2013 and 2014. The CCN concentration over this site showed diurnal variations of high values during nighttime and low values during daytime in association with the change in mesoscale circulation patterns. The inter-annual variations of CCN (CCN0.4% = 2,232 ± 672 cm−3 during August 2013 and CCN0.4% = 941 ± 325 cm−3 during August 2014) are mostly associated with the varying intensity of monsoon rainfall. The variation of CCN number concentration with supersaturation is found to be steeper during nighttime (indicating a less CCN active aerosol system) than during daytime (CCN active system). The CCN activation ratio estimated using simultaneous measurements of CCN and aerosol number (CN) concentration clearly depict the role of land-sea breeze circulations with higher values during daytime than the nighttime. The CCN number concentration predicted for different supersaturations, from measured aerosol number size distribution using Kohler theory, indicate the importance of the change in aerosol composition associated with different airmasses in a coastal environment.

Chemical composition of aerosol particles and light extinction apportionment before and during the heating season in Beijing, China

AbstractDespite extensive efforts into characterization of the sources and formation mechanisms of severe haze pollution in the megacity of Beijing, the response of aerosol composition and optical properties to coal combustion emissions in the heating season remain poorly understood. Here we conducted a 3 month real‐time measurement of submicron aerosol (PM1) composition by an Aerosol Chemical Speciation Monitor and particle light extinction by a Cavity Attenuated Phase Shift extinction monitor in Beijing, China, from 1 October to 31 December 2012. The average (±σ) PM1 concentration was 82.4 (±73.1) µg/m3 during the heating period (HP, 15 November to 31 December), which was nearly 50% higher than that before HP (1 October to 14 November). While nitrate and secondary organic aerosol (SOA) showed relatively small changes, organics, sulfate, and chloride were observed to have significant increases during HP, indicating the dominant impacts of coal combustion sources on these three species. The relative humidity‐dependent composition further illustrated an important role of aqueous‐phase processing for the sulfate enhancement during HP. We also observed great increases of hydrocarbon‐like OA (HOA) and coal combustion OA (CCOA) during HP, which was attributed to higher emissions at lower temperatures and coal combustion emissions, respectively. The relationship between light extinction and chemical composition was investigated using a multiple linear regression model. Our results showed that the largest contributors to particle extinction were ammonium nitrate (32%) and ammonium sulfate (28%) before and during HP, respectively. In addition, the contributions of SOA and primary OA to particle light extinction were quantified. The results showed that the OA extinction was mainly caused by SOA before HP and by SOA and CCOA during HP, yet with small contributions from HOA and cooking aerosol for the entire study period. Our results elucidate substantial changes of aerosol composition, formation mechanisms, and optical properties due to coal combustion emissions and meteorological changes in the heating season.

Aerosol composition, oxidation properties, and sources in Beijing: results from the 2014 Asia-Pacific Economic Cooperation summit study

Abstract. The mitigation of air pollution in megacities remains a great challenge because of the complex sources and formation mechanisms of aerosol particles. The 2014 Asia-Pacific Economic Cooperation (APEC) summit in Beijing serves as a unique experiment to study the impacts of emission controls on aerosol composition, size distributions, and oxidation properties. Herein, a high-resolution time-of-flight aerosol mass spectrometer was deployed in urban Beijing for real-time measurements of size-resolved non-refractory submicron aerosol (NR-PM1) species from 14 October to 12 November 2014, along with a range of collocated measurements. The average (±σ) PM1 was 41.6 (±38.9) μg m−3 during APEC, which was decreased by 53 % compared with that before APEC. The aerosol composition showed substantial changes owing to emission controls during APEC. Secondary inorganic aerosol (SIA: sulfate + nitrate + ammonium) showed significant reductions of 62–69 %, whereas organics presented much smaller decreases (35 %). The results from the positive matrix factorization of organic aerosol (OA) indicated that highly oxidized secondary organic aerosol (SOA) showed decreases similar to those of SIA during APEC. However, primary organic aerosol (POA) from cooking, traffic, and biomass-burning sources were comparable to those before APEC, indicating the presence of strong local source emissions. The oxidation properties showed corresponding changes in response to OA composition. The average oxygen-to-carbon level during APEC was 0.36 (±0.10), which is lower than the 0.43 (±0.13) measured before APEC, demonstrating a decrease in the OA oxidation degree. The changes in size distributions of primary and secondary species varied during APEC. SIA and SOA showed significant reductions in large accumulation modes with peak diameters shifting from ~ 650 to 400 nm during APEC, whereas those of POA remained relatively unchanged. The changes in aerosol composition, size distributions, and oxidation degrees during the aging processes were further illustrated in a case study of a severe haze episode. Our results elucidated a complex response of aerosol chemistry to emission controls, which has significant implications that emission controls over regional scales can substantially reduce secondary particulates. However, stricter emission controls for local source emissions are needed for further mitigating air pollution in the megacity of Beijing.

Real-Time Analysis of Ambient Organic Aerosols Using Aerosol Flowing Atmospheric-Pressure Afterglow Mass Spectrometry (AeroFAPA-MS).

Organic compounds contribute to a major fraction of atmospheric aerosols and have significant impacts on climate and human health. However, because of their chemical complexity, their measurement remains a major challenge for analytical instrumentation. Here we present the development and characterization of a new soft ionization technique that allows mass spectrometric real-time detection of organic compounds in aerosols. The aerosol flowing atmospheric-pressure afterglow (AeroFAPA) ion source is based on a helium glow discharge plasma, which generates excited helium species and primary reagent ions. Ionization of the analytes occurs in the afterglow region after thermal desorption and produces mainly intact quasimolecular ions, facilitating the interpretation of the acquired mass spectra. We illustrate that changes in aerosol composition and concentration are detected on the time scale of seconds and in the ng m(-3) range. Additionally, the successful application of AeroFAPA-MS during a field study in a mixed forest region is presented. In general, the observed compounds are in agreement with previous offline studies; however, the acquisition of chemical information and compound identification is much faster. The results demonstrate that AeroFAPA-MS is a suitable tool for organic aerosol analysis and reveal the potential of this technique to enable new insights into aerosol formation, growth, and transformation in the atmosphere.