Research on the Growth Mechanism of PM2.5 in Central and Eastern China during Autumn and Winter from 2013–2020

Haze is a majorly disastrous type of weather in China, especially central and eastern of China. The development of haze is mainly caused by highly concentrated fine particles (PM2.5) on a regional scale. Here, we present the results from an autumn and winter study conducted from 2013 to 2020 in seven highly polluted areas (27 representative stations) in central and eastern China to analyze the growth mechanism of PM2.5. At the same time, taking Beijing Station as an example, the characteristics of aerosol composition and particle size in the growth phase are analyzed. Taking into account the regional and inter-annual differences of fine particles (PM2.5) distribution, the local average PM2.5 growth value of the year is used as the boundary value for dividing slow, rapid, and explosive growth (only focuses on the hourly growth rate greater than 0). The average value of PM2.5 in the autumn and winter of each regional representative station shows a decreasing trend as a whole, especially after 2017, whereby the decreasing trend was significant. The distribution value of +ΔPM2.5 (PM2.5 hourly growth rate) in the north of the Huai River is lower than that in the south of the Huai River, and both of the +ΔPM2.5 after 2017 showed a significant decreasing trend. The average PM2.5 threshold before the explosive growth is 70.8 µg m−3, and the threshold that is extremely prone to explosive growth is 156 µg m−3 to 277 µg m−3 in north of the Huai River. For the area south of the Huai River, the threshold for PM2.5 explosive growth is relatively low, as a more stringent threshold also puts forward stricter requirements on atmospheric environmental governance. For example, in Beijing, the peak diameters gradually shift to larger sizes when the growth rate increases. The number concentration increasing mainly distributed in Aitken mode (AIM) and Accumulation mode (ACM) during explosive growth. Among the various components of submicron particulate matter (PM1), organic aerosol (OA), especially primary OA (POA), have become one of the most critical components for the PM2.5 explosive growth in Beijing. During the growth period, the contribution of secondary particulate matter (SPM) to the accumulated pollutants is significantly higher than that of primary particulate matter (PPM). However, the proportion of SPM gradually decreases when the growth rate increases. The contribution of the PPM can reach 48% in explosive growth. Compared to slow and rapid growth, explosive growth mainly occurs in the stable atmosphere of higher humidity, lower pressure, lower temperature, small winds, and low mixed layers.

The Emission of VOCs and CO from Heated Tobacco Products, Electronic Cigarettes, and Conventional Cigarettes, and Their Health Risk

The differences in aerosol composition between new tobacco types (heated tobacco products and electronic cigarettes) and conventional cigarettes have not been systematically studied. In this study, the emissions of volatile organic compounds (VOCs), carbon monoxide (CO), nicotine, and tar from heated tobacco products (HTPs), electronic cigarettes (e-cigarettes) and conventional cigarettes were compared, and their health risks were evaluated by applying the same smoking regime and a loss mechanism of smoking. Twenty VOCs were identified in aerosols from HTPs, 18 VOCs were identified in aerosols from e-cigarettes, and 97 VOCs were identified in aerosols from cigarettes by GC–MS and HPLC analysis. The concentrations of total VOCs (TVOCs) emitted by the three types of tobacco products decreased as follows: e-cigarettes (795.4 mg/100 puffs) > cigarettes (83.29 mg/100 puffs) > HTPs (15.65 mg/100 puffs). The nicotine content was 24.63 ± 2.25 mg/100 puffs for e-cigarettes, 22.94 ± 0.03 mg/100 puffs for cigarettes, and 8.817 ± 0.500 mg/100 puffs for HTPs. When using cigarettes of the same brand, the mass concentrations of VOCs, tar, and CO emitted by HTPs were approximately 81.2%, 95.9%, and 97.5%, respectively, lower than the amounts emitted by cigarettes. The health risk results demonstrated that the noncarcinogenic risk of the three types of tobacco products decreased as follows: cigarettes (3609.05) > HTPs (2449.70) > acceptable level (1) > e-cigarettes (0.91). The lifetime cancer risk (LCR) decreased as follows: cigarettes (2.99 × 10−4) > HTPs (9.92 × 10−5) > e-cigarettes (4.80 × 10−5) > acceptable level (10−6). In general, HTPs and e-cigarettes were less harmful than cigarettes when the emission of VOCs and CO was considered.

Identifying Source Region Elemental Indicators in Aged Saharan Dust Plumes Over the Tropical Atlantic

This work examines the spatial dependency of Saharan dust aerosol composition over the Tropical Atlantic Ocean using observations collected during the 2015 Aerosols and Ocean Science Expedition (AEROSE). Regionally specific elemental indicators remain detectable in the dust samples collected along the Saharan air layer trajectory far into the Tropical Atlantic marine boundary layer. Saharan dust transport characteristics and elemental composition were determined by Inductively Coupled Plasma Mass Spectrometric (ICP-MS) analysis of airborne dust samples, ship-based radiometry, satellite aerosol retrievals, and atmospheric back-trajectory analysis. Three strong dust events (SDEs) and two trace dust events (TDEs) were detected during the campaign. The associated mineral dust arrived from potentially 7 different north African countries within 5 to 15 days of emission, according to transport analysis. Peak Na / Al and Ca / Al ratios (>1 and >1.5, respectively) in dust samples were traced to northern Saharan source regions in Western Sahara and Libya. In contrast, peak Fe / Al ratios (0.4–0.8) were traced to surface sources in southern Saharan regions in central Mauritania. We observe the highest ratios of (3–10) at sampling latitudes north of 15N in the Atlantic. Additionally, the sub-micron fraction of dust particulate settling over the Atlantic showed significant temporal and spatial variability, with coarse-fine Al ratios (at 0.8 microns) of 1.05, 0.65, and 0.95 for SDE1 (11/21–23), SDE2 (11/25–26), and SDE3 (11/28), respectively. This was consistent with elemental concentrations of Ca, Na, K, Ti, and Sr, per Al, that exhibited coarser size tendencies per dust event. These observations could validate spatially-sensitive aerosol models by predicting dust aerosol abundance and composition within the tropical Atlantic. Such predictions are critical towards understanding Saharan dust effects on regional climate, Atlantic Ocean biogeochemistry, satellite observations, and air quality modeling.

Source identification of aerosol chemical composition in the Atlas region of North Africa.

<p>Aerosol particles are important constituents of the atmosphere due to their role in controlling climate-related processes. In addition, their impacts on air quality and human health make it essential to study. However, the characterization and the identification of natural and anthropogenic atmospheric particles can be challenging due to the complex mixture occurring during atmospheric transport. Background locations such as high-altitude sites provide valuable infrastructure for obtaining representative data for understanding various pathways for aerosol interactions useful in assessing atmospheric composition. However, information about aerosol characteristics at high-altitude in the African regions and their relation to urban aerosol composition is still not well understood. In the present study, PM<sub>10</sub> and PM<sub>2.5</sub> particulate matter was characterized at two different sites in the North African region of Morocco. A background site located at the newly established AM5 research station in the Middle Atlas region at an altitude of 2100 m and an urban site situated in a polluted city, Fez. The goal was to determine chemical components, evaluate Saharan dust’s role on the PM10 concentrations between the sites, and assess the impact of urban pollution on background aerosol composition. The results indicate that the background aerosol composition is influenced by both regional and trans-regional transport. Despite the site's proximity to the Sahara Desert, the deserts influence on the atmospheric composition was observed for only 22% of the time and this was mainly seasonal. Marine air masses were more dominant with a mixture of sea salt and polluted aerosol from the coastal regions especially during wintertime. Furthermore, high concentrations of mineral dust were observed during the daytime due to the resuspension of road dust. At the same time, an increase of PAHs and anthropogenic metals such as Pb, Ni, and Cu were found during the nighttime because of the boundary layer variation. The Fez's urban site is characterized by a high contribution of elemental carbon (6%) and organic biomass tracers (3%) such as Levoglucosane and 4-nitrophenol.</p>

Sensitivity of Summertime Convection to Aerosol Loading and Properties in the United Arab Emirates

The Weather Research and Forecasting (WRF) model is used to investigate convection–aerosol interactions in the United Arab Emirates (UAE) for a summertime convective event. Both an idealized and climatological aerosol distributions are considered. The convection on 14 August 2013 was triggered by the low-level convergence of the cyclonic circulation associated with the Arabian Heat Low (AHL) and the daytime sea-breeze circulation. Numerical experiments reveal a high sensitivity to aerosol properties. In particular, replacing 20% of the rural aerosols by carbonaceous particles has a comparable impact on the surface radiative fluxes to increasing the aerosol loading by a factor of 10. In both cases, the UAE-averaged net shortwave flux is reduced by ~90 W m−2 while the net longwave flux increases by ~51 W m−2. However, when the aerosol composition is changed, WRF generates 20% more precipitation than when the aerosol loading is increased, due to a broader and weaker AHL. The surface downward and upward shortwave and upward longwave radiation fluxes are found to scale linearly with the aerosol loading. An increase in the amount of aerosols also leads to drier conditions and a delay in the onset of convection due to changes in the AHL.

Urban aerosol chemistry at a land–water transition site during summer – Part 2: Aerosol pH and liquid water content

Particle acidity (aerosol pH) is an important driver of atmospheric chemical processes and the resulting effects on human and environmental health. Understanding the factors that control aerosol pH is critical when enacting control strategies targeting specific outcomes. This study characterizes aerosol pH at a land–water transition site near Baltimore, MD, during summer 2018 as part of the second Ozone Water-Land Environmental Transition Study (OWLETS-2) field campaign. Inorganic fine-mode aerosol composition, gas-phase NH3 measurements, and all relevant meteorological parameters were used to characterize the effects of temperature, aerosol liquid water (ALW), and composition on predictions of aerosol pH. Temperature, the factor linked to the control of NH3 partitioning, was found to have the most significant effect on aerosol pH during OWLETS-2. Overall, pH varied with temperature at a rate of −0.047 K−1 across all observations, though the sensitivity was −0.085 K−1 for temperatures > 293 K. ALW had a minor effect on pH, except at the lowest ALW levels (< 1 µg m−3), which caused a significant increase in aerosol acidity (decrease in pH). Aerosol pH was generally insensitive to composition (SO42-, SO42-:NH4+, total NH3 (Tot-NH3) = NH3 + NH4+), consistent with recent studies in other locations. In a companion paper, the sources of episodic NH3 events (95th percentile concentrations, NH3 > 7.96 µg m−3) during the study are analyzed; aerosol pH was higher by only ∼ 0.1–0.2 pH units during these events compared to the study mean. A case study was analyzed to characterize the response of aerosol pH to nonvolatile cations (NVCs) during a period strongly influenced by primary Chesapeake Bay emissions. Depending on the method used, aerosol pH was estimated to be either weakly (∼ 0.1 pH unit change based on NH3 partitioning calculation) or strongly (∼ 1.4 pH unit change based on ISORROPIA thermodynamic model predictions) affected by NVCs. The case study suggests a strong pH gradient with size during the event and underscores the need to evaluate assumptions of aerosol mixing state applied to pH calculations. Unique features of this study, including the urban land–water transition site and the strong influence of NH3 emissions from both agricultural and industrial sources, add to the understanding of aerosol pH and its controlling factors in diverse environments.

First insights into northern Africa high-altitude background aerosol chemical composition and source influences

Field measurements were conducted to determine aerosol chemical composition at a newly established remote high-altitude site in North Africa at the Atlas Mohammed V (AMV) atmospheric observatory located in the Middle Atlas Mountains. The main objectives of the present work are to investigate the variations in the aerosol composition and better assess global and regional changes in atmospheric composition in North Africa. A total of 200 particulate matter (PM10) filter samples were collected at the site using a high-volume (HV) collector in a 12 h sampling interval from August to December 2017. The chemical composition of the samples was analyzed for trace metals, water-soluble ions, organic carbon (OC/EC), aliphatic hydrocarbons, and polycyclic aromatic hydrocarbon (PAH) contents. The results indicate that high-altitude aerosol composition is influenced by both regional and transregional transport of emissions. However, local sources play an important role, especially during low wind speed periods, as observed for November and December. During background conditions characterized by low wind speeds (avg. 3 m s-1) and mass concentrations in the range from 9.8 to 12 μg m-3, the chemical composition is found to be dominated by inorganic elements, mainly suspended dust (61 %) and ionic species (7 %), followed by organic matter (7 %), water content (12 %), and unidentified mass (11 %). Despite the proximity of the site to the Sahara, its influence on the atmospheric composition at this high-altitude site was mainly seasonal and accounted for only 22 % of the sampling duration. Biogenic organics contributed up to 7 % of the organic matter with high contributions from compounds such as heneicosane, hentriacontane, and nonacosane. The AMV site is dominated by four main air mass inflows, which often leads to different aerosol chemical compositions. Mineral dust influence was seasonal and ranged between 21 % and 74 % of the PM mass, with peaks observed during the summer, and was accompanied by high concentrations of SO42- of up to 3.0 μg m-3. During winter, PM10 concentrations are low (<30 μg m-3), the influence of the desert is weaker, and the marine air masses (64 %) are more dominant with a mixture of sea salt and polluted aerosol from the coastal regions (Rabat and Casablanca). During the daytime, mineral dust contribution to PM increased by about 42 % because of road dust resuspension. In contrast, during nighttime, an increase in the concentrations of alkanes, PAHs, alkane-2-ones, and anthropogenic metals such as Pb, Ni, and Cu was found due to variations in the boundary layer height. The results provide the first detailed seasonal and diurnal variation of the aerosol chemical composition, which is valuable for long-term assessment of climate and regional influence of air pollution in North Africa.

Transport-driven aerosol differences above and below the canopy of a mixed deciduous forest

Exchanges of energy and mass between the surrounding air and plant surfaces occur below, within, and above a forest's vegetative canopy. The canopy also can lead to vertical gradients in light, trace gases, oxidant availability, turbulent mixing, and properties and concentrations of organic aerosol (OA). In this study, a high-resolution time-of-flight aerosol mass spectrometer was used to measure non-refractory submicron aerosol composition and concentration above (30 m) and below (6 m) a forest canopy in a mixed deciduous forest at the Program for Research on Oxidants: PHotochemistry, Emissions, and Transport tower in northern Michigan during the summer of 2016. Three OA factors are resolved using positive matrix factorization: more-oxidized oxygenated organic aerosol (MO-OOA), isoprene-epoxydiol-derived organic aerosol (IEPOX-OA), and 91Fac (a factor characterized with a distinct fragment ion at m/z 91) from both the above- and the below-canopy inlets. MO-OOA was most strongly associated with long-range transport from more polluted regions to the south, while IEPOX-OA and 91Fac were associated with shorter-range transport and local oxidation chemistry. Overall vertical similarity in aerosol composition, degrees of oxidation, and diurnal profiles between the two inlets was observed throughout the campaign, which implies that rapid in-canopy transport of aerosols is efficient enough to cause relatively consistent vertical distributions of aerosols at this scale. However, four distinct vertical gradient episodes are identified for OA, with vertical concentration differences (above-canopy minus below-canopy concentrations) in total OA of up to 0.8 µg m−3, a value that is 42 % of the campaign average OA concentration of 1.9 µg m−3. The magnitude of these differences correlated with concurrent vertical differences in either sulfate aerosol or ozone. These differences are likely driven by a combination of long-range transport mechanisms, canopy-scale mixing, and local chemistry. These results emphasize the importance of including vertical and horizontal transport mechanisms when interpreting trace gas and aerosol data in forested environments.