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Showing papers on "Particulates published in 2019"


Journal ArticleDOI
TL;DR: The data show independent associations between short-term exposure to PM10 and PM2.5 and daily all-cause, cardiovascular, and respiratory mortality in more than 600 cities across the globe, and reinforce the evidence of a link between mortality and PM concentration established in regional and local studies.
Abstract: BACKGROUND: The systematic evaluation of the results of time-series studies of air pollution is challenged by differences in model specification and publication bias.METHODS: We evaluated the assoc ...

896 citations


Journal ArticleDOI
TL;DR: In this paper, the authors show observational evidence for this effect with 2013-2018 summer data of hourly ozone and PM2.5 concentrations from 106 sites in the North China Plain.
Abstract: Fine particulate matter (PM2.5) decreased by 30–40% across China during 2013–2017 in response to the governmental Clean Air Action. However, surface ozone pollution worsened over the same period. Model simulations have suggested that the increase in ozone could be driven by the decrease in PM2.5, because PM2.5 scavenges hydroperoxy (HO2) and NOx radicals that would otherwise produce ozone. Here we show observational evidence for this effect with 2013–2018 summer data of hourly ozone and PM2.5 concentrations from 106 sites in the North China Plain. The observations show suppression of ozone pollution at high PM2.5 concentrations, consistent with a model simulation in which PM2.5 scavenging of HO2 and NOx depresses ozone concentrations by 25 ppb relative to PM2.5-free conditions. PM2.5 chemistry makes ozone pollution less sensitive to NOx emission controls, emphasizing the need for controlling emissions of volatile organic compounds (VOCs), which so far have not decreased in China. The new 2018–2020 Clean Air Action plan calls for a 10% decrease in VOC emissions that should begin to reverse the long-term ozone increase even as PM2.5 continues to decrease. Aggressive reduction of NOx and aromatic VOC emissions should be particularly effective for decreasing both PM2.5 and ozone. Observations confirm that cleaning up fine particulate matter in the North China Plain has exacerbated ozone pollution, suggesting that both NOx and VOC emissions need to be reduced to improve air quality.

411 citations


Journal ArticleDOI
TL;DR: This work develops geoscience-derived estimates of PM2.5 composition from a chemical transport model and satellite observations of aerosol optical depth and statistically fuse these estimates with ground-based observations using a geographically weighted regression over North America to produce a spatially complete representation.
Abstract: An accurate fine-resolution surface of the chemical composition of fine particulate matter (PM2.5) would offer valuable information for epidemiological studies and health impact assessments. We develop geoscience-derived estimates of PM2.5 composition from a chemical transport model (GEOS-Chem) and satellite observations of aerosol optical depth, and statistically fuse these estimates with ground-based observations using a geographically weighted regression over North America to produce a spatially complete representation of sulfate, nitrate, ammonium, black carbon, organic matter, mineral dust, and sea-salt over 2000-2016. Significant long-term agreement is found with cross-validation sites over North America (R2 = 0.57-0.96), with the strongest agreement for sulfate (R2 = 0.96), nitrate (R2 = 0.90), and ammonium (R2 = 0.86). We find that North American decreases in population-weighted fine particulate matter (PM2.5) concentrations since 2000 have been most heavily influenced by regional changes in sulfate and organic matter. Regionally, the relative importance of several chemical components are found to change with PM2.5 concentration, such as higher PM2.5 concentrations having a larger proportion of nitrate and a smaller proportion of sulfate. This data set offers information for research into the health effects of PM2.5 chemical components.

406 citations


Journal ArticleDOI
TL;DR: Evidence of black carbon particle deposition on the fetal side of human placentae, including at early stages of pregnancy, is reported, suggesting air pollution could affect birth outcome through direct effects on the fetus.
Abstract: Particle transfer across the placenta has been suggested but to date, no direct evidence in real-life, human context exists. Here we report the presence of black carbon (BC) particles as part of combustion-derived particulate matter in human placentae using white-light generation under femtosecond pulsed illumination. BC is identified in all screened placentae, with an average (SD) particle count of 0.95 × 104 (0.66 × 104) and 2.09 × 104 (0.9 × 104) particles per mm3 for low and high exposed mothers, respectively. Furthermore, the placental BC load is positively associated with mothers’ residential BC exposure during pregnancy (0.63–2.42 µg per m3). Our finding that BC particles accumulate on the fetal side of the placenta suggests that ambient particulates could be transported towards the fetus and represents a potential mechanism explaining the detrimental health effects of pollution from early life onwards. Exposure to air pollution during pregnancy has been associated with impaired birth outcomes. Here, Bove et al. report evidence of black carbon particle deposition on the fetal side of human placentae, including at early stages of pregnancy, suggesting air pollution could affect birth outcome through direct effects on the fetus.

333 citations


Journal ArticleDOI
TL;DR: Particulate plastics made of synthetic polymers, their origin, and characteristics are described with emphasis on how particulate plastics and associated toxic trace elements contaminate terrestrial and aquatic ecosystems.

298 citations


Journal ArticleDOI
TL;DR: The pathophysiology to support the epidemiologic associations between mortality and morbidity and ozone centers at the chemical and toxicological property of ozone as a strong oxidant, being able to induce oxidative damages to cells and the lining fluids of the airways, and immune-inflammatory responses within and beyond the lung.
Abstract: Oxides of nitrogen (NOx) and volatile organic compounds (VOCs) released into the atmosphere can react in the presence of solar irradiation, leading to ozone formation in the troposphere. Historically, before clean air regulations were implemented to control NOx and VOCs, ozone concentrations were high enough to exert acute effects such as eye and nose irritation, respiratory disease emergencies, and lung function impairment. At or above current regulatory standards, day-to-day variations in ozone concentrations have been positively associated with asthma incidence and daily non-accidental mortality rate. Emerging evidence has shown that both short-term and long-term exposures to ozone, at concentrations below the current regulatory standards, were associated with increased mortality due to respiratory and cardiovascular diseases. The pathophysiology to support the epidemiologic associations between mortality and morbidity and ozone centers at the chemical and toxicological property of ozone as a strong oxidant, being able to induce oxidative damages to cells and the lining fluids of the airways, and immune-inflammatory responses within and beyond the lung. These new findings add substantially to the existing challenges in controlling ozone pollution. For example, in the United States in 2016, 90% of non-compliance to the national ambient air quality standards was due to ozone whereas only 10% was due to particulate matter and other regulated pollutants. Climate change, through creating atmospheric conditions favoring ozone formation, has been and will continue to increase ozone concentrations in many parts of world. Worldwide, ozone is responsible for several hundreds of thousands of premature deaths and tens of millions of asthma-related emergency room visits annually. To combat ozone pollution globally, more aggressive reductions in fossil fuel consumption are needed to cut NOx and VOCs as well as greenhouse gas emissions. Meanwhile, preventive and therapeutic strategies are needed to alleviate the detrimental effects of ozone especially in more susceptible individuals. Interventional trials in humans are needed to evaluate the efficacy of antioxidants and ozone-scavenging compounds that have shown promising results in animal studies.

280 citations


Journal ArticleDOI
TL;DR: Modeling of particle deposition in the human lung indicated that coarse particles generated by crustal sources may have adverse health effects as strong as those resulting from fine particles generated from combustion sources.

167 citations


Journal ArticleDOI
TL;DR: This analysis showed significant associations between short-term PM2.5–10 exposure and daily nonaccidental and cardiopulmonary mortality based on data from 272 cities located throughout China.
Abstract: Background: Coarse particulate matter with aerodynamic diameter between 2.5 and 10μm (PM2.5–10) air pollution is a severe environmental problem in developing countries, but its challenges to public...

139 citations


Journal ArticleDOI
TL;DR: In this paper, the authors report on 1.25 years of highly time-resolved speciated submicron particulate matter (PM 1 ) data, including black carbon (BC) and non-refractory PM 1 (NR-PM 1 ), which they combine to develop a composition-based estimate of PM 1.
Abstract: . Delhi, India, routinely experiences some of the world's highest urban particulate matter concentrations. We established the Delhi Aerosol Supersite study to provide long-term characterization of the ambient submicron aerosol composition in Delhi. Here we report on 1.25 years of highly time-resolved speciated submicron particulate matter (PM 1 ) data, including black carbon (BC) and nonrefractory PM 1 (NR-PM 1 ), which we combine to develop a composition-based estimate of PM 1 (“C-PM 1 ” = BC + NR-PM 1 ) concentrations. We observed marked seasonal and diurnal variability in the concentration and composition of PM 1 owing to the interactions of sources and atmospheric processes. Winter was the most polluted period of the year, with average C-PM 1 mass concentrations of ∼210 µ g m −3 . The monsoon was hot and rainy, consequently making it the least polluted (C-PM 1 ∼50 µ g m −3 ) period. Organics constituted more than half of the C-PM 1 for all seasons and times of day. While ammonium, chloride, and nitrate each were ∼10 % of the C-PM 1 for the cooler months, BC and sulfate contributed ∼5 % each. For the warmer periods, the fractional contribution of BC and sulfate to C-PM 1 increased, and the chloride contribution decreased to less than 2 %. The seasonal and diurnal variation in absolute mass loadings were generally consistent with changes in ventilation coefficients, with higher concentrations for periods with unfavorable meteorology – low planetary boundary layer height and low wind speeds. However, the variation in C-PM 1 composition was influenced by temporally varying sources, photochemistry, and gas–particle partitioning. During cool periods when wind was from the northwest, episodic hourly averaged chloride concentrations reached 50–100 µ g m −3 , ranking among the highest chloride concentrations reported anywhere in the world. We estimated the contribution of primary emissions and secondary processes to Delhi's submicron aerosol. Secondary species contributed almost 50 %–70 % of Delhi's C-PM 1 mass for the winter and spring months and up to 60 %–80 % for the warmer summer and monsoon months. For the cooler months that had the highest C-PM 1 concentrations, the nighttime sources were skewed towards primary sources, while the daytime C-PM 1 was dominated by secondary species. Overall, these findings point to the important effects of both primary emissions and more regional atmospheric chemistry on influencing the extreme particle concentrations that impact the Delhi megacity region. Future air quality strategies considering Delhi's situation in both a regional and local context will be more effective than policies targeting only local, primary air pollutants.

129 citations


Journal ArticleDOI
TL;DR: The results of a health risk assessment indicated that the incremental lifetime cancer risk forPeople in the northern cities was higher than that for people in the other regions, especially during the cold season, and the potential risk of airborne particulate PAH exposure was relatively high in some cities.

123 citations


Journal ArticleDOI
TL;DR: This review examines current knowledge regarding the sources of vehicle-derived Fe-bearing nanoparticles, their chemical and mineralogical compositions, grain size distribution, and potential hazard to human health.
Abstract: Airborne particulate matter poses a serious threat to human health. Exposure to nanosized (<0.1 μm), vehicle-derived particulates may be hazardous due to their bioreactivity, their ability to penet...

Journal ArticleDOI
TL;DR: It is shown that NO2 measurements from the new, high-resolution TROPOMI satellite sensor can directly determine the strength and distribution of emissions from Paris, and suggest that Paris emissions in 2018 are only 5–15% below inventory estimates for 2011–2012, reflecting the difficulty of meeting NOx emission reduction targets.
Abstract: Nitrogen dioxide (NO2) is a regulated air pollutant that is of particular concern in many cities, where concentrations are high. Emissions of nitrogen oxides to the atmosphere lead to the formation of ozone and particulate matter, with adverse impacts on human health and ecosystems. The effects of emissions are often assessed through modeling based on inventories relying on indirect information that is often outdated or incomplete. Here we show that NO2 measurements from the new, high-resolution TROPOMI satellite sensor can directly determine the strength and distribution of emissions from Paris. From the observed build-up of NO2 pollution, we find highest emissions on cold weekdays in February 2018, and lowest emissions on warm weekend days in spring 2018. The new measurements provide information on the spatio-temporal distribution of emissions within a large city, and suggest that Paris emissions in 2018 are only 5–15% below inventory estimates for 2011–2012, reflecting the difficulty of meeting NOx emission reduction targets.

Journal ArticleDOI
Yong Qian1, Zilong Li1, Liang Yu1, Xiaole Wang1, Xingcai Lu1 
TL;DR: In this article, a comprehensive review on the latest research progress, including the particulate matter formation mechanism of gasoline engines, effects of fuel/air mixture preparation strategies, fuel physical-chemical properties, and engine operating conditions on particulate size distribution characteristics, and the effects of the driving cycle on vehicle particulate emissions were summarized.

Journal ArticleDOI
TL;DR: This review summarizes available observations of aging-related biomass burning aerosol mass concentrations and composition markers, and discusses four broad hypotheses to explain variability within and between field and laboratory campaigns.
Abstract: Biomass burning is a major source of atmospheric particulate matter (PM) with impacts on health, climate, and air quality. The particles and vapors within biomass burning plumes undergo chemical and physical aging as they are transported downwind. Field measurements of the evolution of PM with plume age range from net decreases to net increases, with most showing little to no change. In contrast, laboratory studies tend to show significant mass increases on average. On the other hand, similar effects of aging on the average PM composition (e.g., oxygen-to-carbon ratio) are reported for lab and field studies. Currently, there is no consensus on the mechanisms that lead to these observed similarities and differences. This review summarizes available observations of aging-related biomass burning aerosol mass concentrations and composition markers, and discusses four broad hypotheses to explain variability within and between field and laboratory campaigns: (1) variability in emissions and chemistry, (2) differences in dilution/entrainment, (3) losses in chambers and lines, and (4) differences in the timing of the initial measurement, the baseline from which changes are estimated. We conclude with a concise set of research needs for advancing our understanding of the aging of biomass burning aerosol.

Journal ArticleDOI
TL;DR: In this article, the results of studies of the integral toxicity of exhaust gases of a diesel engine operating on natural gas and alcohol emulsions are presented, and the regimes characterizing the specific toxicity of diesel engine under its operating conditions were determined, and emissions of toxic components on these regimes were determined taking into account their weight coefficients.
Abstract: The results of studies of the integral toxicity of exhaust gases of a diesel engine operating on natural gas and alcohol emulsions are presented. At the same time, the regimes characterizing the specific toxicity of a diesel engine under its operating conditions were determined, and emissions of toxic components on these regimes were determined taking into account their weight coefficients. The results of research specific toxic diesel exhaust toxicity indicators, in accordance with the requirements of UNECE Regulation No. 49, show that when a diesel engine operates on natural gas with exhaust gas recirculation and an ethanol-fuel emulsion, the content of nitrogen oxides (NOx) and carbon dioxide (CO) in the exhaust gases conforms to "EURO 3", particulate matter – "EURO 5", total hydrocarbons (CHx) – "EURO 2". When the diesel engine is running on a methanol-fuel emulsion, the content of NOx, СНx and CO in the exhaust gases complies with the standards "EURO 3", particulate matter – "EURO 5".

Journal ArticleDOI
TL;DR: Overall, few consistent associations were observed between the different air pollution measures and IHD or stroke incidence, however, long-term residential exposure to locally emitted BC from traffic exhaust was associated with stroke incidence.
Abstract: BACKGROUND: Long-term exposure to particulate matter (PM) in ambient air has been associated with cardiovascular mortality, but few studies have considered incident disease in relation to PM from d ...

Journal ArticleDOI
TL;DR: In this article, the authors present evidence of primary sulfate emissions from residential coal combustion (RCC) by testing particulate matter (PM) emissions from briquettes and chunk coal burned in a household stove.

Journal ArticleDOI
TL;DR: Most of the OSA that formed in this process remained in the water column, where the degradation processes were more effective, and there was no evidence of the transport of hydrocarbons in bottom sediments associated with fine sediments that would have accelerated the dispersion and degradation rates of the oil.
Abstract: This paper presents the oil-suspended particulate matter aggregate (OSA) resulted from the interaction of droplets of dispersed oil in a water column and particulate matter. This structure reduces the adhesion of oil on solid surfaces, promotes dispersion, and may accelerate degradation processes. The effects of the addition of fine sediments (clay + silt) on the formation of OSA, their impact on the dispersion and degradation of the oil, and their potential use in recovering reflective sandy beaches were evaluated in a mesoscale simulation model. Two simulations were performed (21 days), in the absence and presence of fine sediments, with four units in each simulation using oil from the Reconcavo Basin. The results showed that the use of fine sediment increased the dispersion of the oil in the water column up to four times in relation to the sandy sediment. There was no evidence of the transport of hydrocarbons in bottom sediments associated with fine sediments that would have accelerated the dispersion and degradation rates of the oil. Most of the OSA that formed in this process remained in the water column, where the degradation processes were more effective. Over the 21 days of simulation, we observed a 40 % reduction on average of the levels of saturated hydrocarbons staining the surface oil.

Journal ArticleDOI
TL;DR: There is little direct evidence that underground railway particulate matter exposure is more harmful than ambient particulate Matter exposure, and future research should focus on outcomes of chronic in vivo exposure, as well as further work to understand mechanisms and potential biomarkers of exposure.
Abstract: Exposure to ambient airborne particulate matter is a major risk factor for mortality and morbidity, associated with asthma, lung cancer, heart disease, myocardial infarction, and stroke, and more recently type 2 diabetes, dementia and loss of cognitive function. Less is understood about differential effects of particulate matter from different sources. Underground railways are used by millions of people on a daily basis in many cities. Poor air exchange with the outside environment means that underground railways often have an unusually high concentration of airborne particulate matter, while a high degree of railway-associated mechanical activity produces particulate matter which is physicochemically highly distinct from ambient particulate matter. The implications of this for the health of exposed commuters and employees is unclear. A literature search found 27 publications directly assessing the potential health effects of underground particulate matter, including in vivo exposure studies, in vitro toxicology studies, and studies of particulate matter which might be similar to that found in underground railways. The methodology, findings, and conclusions of these studies were reviewed in depth, along with further publications directly relevant to the initial search results. In vitro studies suggest that underground particulate matter may be more toxic than exposure to ambient/urban particulate matter, especially in terms of endpoints related to reactive oxygen species generation and oxidative stress. This appears to be predominantly a result of the metal-rich nature of underground particulate matter, which is suggestive of increased health risks. However, while there are measureable effects on a variety of endpoints following exposure in vivo, there is a lack of evidence for these effects being clinically significant as may be implied by the in vitro evidence. There is little direct evidence that underground railway particulate matter exposure is more harmful than ambient particulate matter exposure. This may be due to disparities between in vivo exposures and in vitro models, and differences in exposure doses, as well as statistical under powering of in vivo studies of chronic exposure. Future research should focus on outcomes of chronic in vivo exposure, as well as further work to understand mechanisms and potential biomarkers of exposure.

Journal ArticleDOI
TL;DR: This study attempted to explore the toxicity contribution and combined effects of PM-bounded metals in human lung epithelial cells (A549), and highlighted the potential contribution from heavy metals and their interactions to PM toxicity, and promoted the application of toxicity prediction models.

Journal ArticleDOI
01 Mar 2019
TL;DR: Wide changes associated with aerosol loadings, humidity, and vertical advection patterns with displacements of major trace and greenhouse gasses are observed, all of which can have significant ramifications in terms of human health and changes in weather pattern.
Abstract: The northern part of India, adjoining the Himalaya, is considered as one of the global hot spots of pollution because of various natural and anthropogenic factors. Throughout the year, the region is affected by pollution from various sources like dust, biomass burning, industrial and vehicular pollution, and myriad other anthropogenic emissions. These sources affect the air quality and health of millions of people who live in the Indo-Gangetic Plains. The dust storms that occur during the premonsoon months of March-June every year are one of the principal sources of pollution and originate from the source region of Arabian Peninsula and the Thar desert located in north-western India. In the year 2018, month of May, three back-to-back major dust storms occurred that caused massive damage, loss of human lives, and loss to property and had an impact on air quality and human health. In this paper, we combine observations from ground stations, satellites, and radiosonde networks to assess the impact of dust events in the month of May 2018, on meteorological parameters, aerosol properties, and air quality. We observed widespread changes associated with aerosol loadings, humidity, and vertical advection patterns with displacements of major trace and greenhouse gasses. We also notice drastic changes in suspended particulate matter concentrations, all of which can have significant ramifications in terms of human health and changes in weather pattern.

Journal ArticleDOI
TL;DR: In this paper, a review summarizes the evolution of PM mass emissions from gasoline vehicles placed in the market from early 1990s until 2019 in different parts of the world, and the analysis then extends to total and nonvolatile particle number emissions.
Abstract: The particulate matter (PM) emissions of gasoline vehicles were much lower than those of diesel vehicles until the introduction of diesel particulate filters (DPFs) in the early 2000s. At the same time, gasoline direct injection (GDI) engines started to become popular in the market due to their improved efficiency over port fuel injection (PFI) ones. However, the PM mass and number emissions of GDI vehicles were higher than their PFI counterparts and diesel ones equipped with DPFs. Stringent PM mass levels and the introduction of particle number limits for GDI vehicles in the European Union (EU) resulted in significant PM reductions. The EU requirement to fulfill the proposed limits on the road resulted to the introduction of gasoline particulate filters (GPFs) in EU GDI models. This review summarizes the evolution of PM mass emissions from gasoline vehicles placed in the market from early 1990s until 2019 in different parts of the world. The analysis then extends to total and nonvolatile particle number emissions. Care is given to reveal the impact of ambient temperature on emission levels. The discussion tries to provide scientific input to the following policy-relevant questions. Whether particle number limits should be extended to gasoline PFI vehicles, whether the lower limit of 23 nm for particle number measurements should be decreased to 10 nm, and whether low ambient temperature tests for PM should be included.

Journal ArticleDOI
Jiangping Chen1, Jianhua Yin1, Lin Zang1, Taixin Zhang1, Mengdi Zhao1 
TL;DR: A stacking model was developed, which contained three submodels of machine learning, namely, AdaBoost, XGBoost and random forest, stacked through a multiple linear regression model and showed that the proposed stacking model performed better than the single models when applied to the test set.

Journal ArticleDOI
TL;DR: In this paper, the authors investigated the PFAS contamination in the coastal areas of Shandong Province and revealed the partition behaviors of PFAS in the water-SPM system and water-sediment system.

Journal ArticleDOI
TL;DR: In this article, the authors proposed a total environmental impact score (TEIS) approach to assess the environmental impact of the main industrial processes of an integrated iron and steel site located in the northeast of China.

Journal ArticleDOI
TL;DR: This cohort study provided the first evidence from China that long-term exposure to PM2.5 was independently associated with incident hypertension at relatively high ambient concentrations.
Abstract: The risk of incident hypertension associated with long-term exposure to fine particulate matter (PM2.5) was still unclear by studies conducted in North America and Europe, and this relationship has...

Journal ArticleDOI
TL;DR: It is demonstrated that the leachable fraction of particle-bound As, Pb, Cr, Mn, Cd, Cu, Ni and Zn in lung fluid within the typical retention duration of particles in human lungs varied drastically among particles originated from different air pollution sources.

Journal ArticleDOI
TL;DR: Different chemical responses of aerosol species to emission changes and meteorology are highlighted, suggesting that future mitigation of air pollution in China needs species-targeted control policy.

Journal ArticleDOI
TL;DR: The rate of dust accumulation reaches approximately 40 mg m−m−2day−1 in the no-precipitation period and it was at least two times higher than fluxes calculated on the basis of PM10 and TSP concentrations which suggest that additional forces such as electrostatic forces significantly influence dust deposition.
Abstract: Solid particles impair the performance of the photovoltaic (PV) modules. This results in power losses which lower the efficiency of the system as well as the increases of temperature which additionally decreases the performance and lifetime. The deposited dust chemical composition, concentration and formation of a dust layer on the PV surface differ significantly in reference to time and location. In this study, an evaluation of dust deposition on the PV front cover glass during the non-heating season in one of the most polluted European cities, Krakow, was performed. The time-dependent particle deposition and its correlation to the air pollution with particulate matter were analysed. Dust deposited on several identical PV modules during variable exposure periods (from 1 day up to 1 week) and the samples of total suspended particles (TSP) on quartz fibre filters using a low volume sampler were collected during the non-heating season in the period of 5 weeks. The concentration of TSP in the study period ranged between 12.5 and 60.05 μg m−3 while the concentration of PM10 observed in the Voivodeship Inspectorate of Environmental Protection traffic station, located 1.2 km from the TSP sampler, ranged from 14 to 47 μg m−3. It was revealed that dust deposition density on a PV surface ranged from 7.5 to 42.1 mg m−2 for exposure periods of 1 day while the measured weekly dust deposition densities ranged from 25.8 to 277.0 mg m−2. The precipitation volume and its intensity as well as humidity significantly influence the deposited dust. The rate of dust accumulation reaches approximately 40 mg m−2day−1 in the no-precipitation period and it was at least two times higher than fluxes calculated on the basis of PM10 and TSP concentrations which suggest that additional forces such as electrostatic forces significantly influence dust deposition.

Journal ArticleDOI
TL;DR: The observed diel cycle of aerosol phase should provoke rethinking of the SOA atmospheric lifecycle, as it suggests diurnal variability in gas-particle partitioning and mixing time scales, which influence aerosol multiphase chemistry, lifetime, and climate impacts.
Abstract: Aerosol phase state is critical for quantifying aerosol effects on climate and air quality. However, significant challenges remain in our ability to predict and quantify phase state during its evolution in the atmosphere. Herein, we demonstrate that aerosol phase (liquid, semisolid, solid) exhibits a diel cycle in a mixed forest environment, oscillating between a viscous, semisolid phase state at night and liquid phase state with phase separation during the day. The viscous nighttime particles existed despite higher relative humidity and were independently confirmed by bounce factor measurements and atomic force microscopy. High-resolution mass spectrometry shows the more viscous phase state at night is impacted by the formation of terpene-derived and higher molecular weight secondary organic aerosol (SOA) and smaller inorganic sulfate mass fractions. Larger daytime particulate sulfate mass fractions, as well as a predominance of lower molecular weight isoprene-derived SOA, lead to the liquid state of the daytime particles and phase separation after greater uptake of liquid water, despite the lower daytime relative humidity. The observed diel cycle of aerosol phase should provoke rethinking of the SOA atmospheric lifecycle, as it suggests diurnal variability in gas-particle partitioning and mixing time scales, which influence aerosol multiphase chemistry, lifetime, and climate impacts.