Aged Aerosol Research Articles

Исследование методов и современных технических решений очистки аэрозольных выбросов промышленности

The analysis and characterization of aerosol emissions into the atmosphere are given, the ways of formation of primary and secondary aerosols are considered. The process of atmospheric aging of aerosols, which has a negative impact on the environment, is considered. The functional links between aerosol emissions, their source and impact on climate and public health are presented. The possible influence of the reactions of liquid and solid aerosol particles on the properties of atmospheric air is considered. The main methods of purification of industrial aerosol emissions are considered: adsorption purification, thermal and catalytic neutralization, chemisorption and absorption purification. The ways of increasing the efficiency of adsorption processes, for example, the separation of adsorbent in the apparatus, are analyzed. The essence of the process of thermal neutralization of gas mixtures is described, it is established that thermal installations based on the direct combustion method work more efficiently when combining thermal and catalytic neutralization methods, designs of combined equipment are presented, and ways to increase the intensity of the apparatus are considered. The process of gas purification based on the absorption process is considered. It is determined that absorption plants for cleaning gases from harmful components are the most effective and efficient due to the high level of technical implementation of the process. The development and improvement of the main absorber equipment is aimed at achieving maximum cleaning efficiency with an optimal pressure drop that determines energy consumption. The analysis shows the negative impact of natural and anthropogenic aerosols on the environment. In order to correctly solve the problem, information on the sources, composition and properties of aerosols is needed to select the most effective and economically profitable cleaning method, which will help reduce the anthropogenic load on the atmosphere.

Evidence for Cytotoxicity and Mitochondrial Dysfunction in Human Lung Cells Exposed to Biomass Burning Aerosol Constituents: Levoglucosan and 4-Nitrocatechol

Biomass burning (BB) emissions are one of the largest sources of carbonaceous aerosol, posing a significant risk as an airway irritant. Important BB markers include wood pyrolysis emissions, such as levoglucosan (LG) that is an anhydrous sugar bearing a six-carbon ring structure (i.e., 1,6-anhydro-β-D-glucopyranose). Atmospheric chemical aging of BB-derived aerosol (BBA) in the presence of nitrogen oxides (NOx) can yield nitro-aromatic compounds, including 4-nitrocatechol (4NC). There is building evidence that NOx-mediated chemical aging of BBA poses a more serious exposure effect than primary pyrolysis emissions. This study provides a comparative toxicological assessment following the exposure to important BBA marker compounds in human lung cells (i.e., A549 and BEAS-2B) to determine whether aromatic 4NC is more toxic than BBA-bound anhydrous carbohydrate (i.e., LG). We determined inhibitory concentration-50 (IC50) and examined reactive oxygen species (ROS) changes, mitochondrial dysfunction, and apoptosis induction in the two cell lines following exposure to LG and 4NC in a dose-response manner. In the BEAS-2B cells, estimated IC50 values for 4NC were 33 and 8.8 μg mL-1, and for LG were 2546 and ∼ 3 × 107 μg mL-1 at 24 h and 48 h of exposure, respectively. A549 cells exhibited a much higher IC50 value than BEAS-2B cells. LG exposures resulted in mitochondrial stress with viability inhibition, but cells recovered with increasing exposure time. 4NC exposures at 200 μg mL-1 resulted in the induction of apoptosis at 6 h. Mitochondrial dysfunction and ROS imbalance induced the intrinsic apoptotic pathway induction following 4NC exposures. While increased ROS is caused by LG exposure in lung cells, 4NC is a marker of concern during BB emissions, as we observed apoptosis and high mitochondrial ROS in both lung cells at atmospherically-relevant aerosol concentrations. It may be associated with higher airway or inhalation pathologies in higher BBA emissions, such as wildfires or during wood combustion.

Insights into chemical aging of urban aerosols over Delhi, India

Atmospheric particles can undergo aging as they are transported over long distances and mix with particles from other sources. This can lead to the accumulation of pollutants and the formation of complex aerosol mixtures with diverse chemical and physical properties. To investigate the process of aging in ambient atmosphere, 24h sampling of PM2.5 aerosol particles on Quartz microfiber filter with a tin substrate was carried out from November 2020 to March 2021 at CSIR-National Physical Laboratory, New Delhi (28°38'10″ N and 77°10′17" E), using fine particle sampler. Based on the observations of weather and meteorological parameters, a few episodic cases have been selected, and samples were analyzed at bulk and individual particle level. The objective of the present study is to investigate the aging characteristics of aerosols, enabling us to understand the mixing of aerosols (at both bulk and individual particle levels) and the variation in fresh and deformed (aged with other species) graphitic content in the episodic cases. The Raman Spectroscopy technique employed measures the intensity of graphitic (G band; around 1580 cm−1) and disordered graphitic (D band; around 1320 cm−1) content of aerosols. Individual particle microscopic observations reveal the occurrence of open chain fractals of black carbon in variable monomer sizes, sometimes agglomerated with metals like Cu, Cr, Ca etc., along with the presence of S- rich and organic aerosols while the Raman Spectrum (bulk sample analysis) highlights graphitic and disordered (when graphite interacts with other chemical species) graphitic intensities. Comparing the intensities of heavy haze and moderate haze with non-haze days (for comparison purpose, March 23, 2021 with the lowest PM2.5 concentration ∼ 62 μg/m3, has been considered as a non-haze day), it was observed that the intensities recorded on haze days were 45 to 200 times higher for the G band and 43 to 93 times higher for the D band; while for moderate haze days, the intensities were 4 to 61 times higher for the G band and 2 to 29 times higher for the D band. These findings suggest chemical processing of BC during haze days.

Imaging Dissolution Dynamics of Individual NaCl Nanoparticles during Deliquescence with In Situ Transmission Electron Microscopy.

Water vapor condensation on hygroscopic aerosol particles plays an important role in cloud formation, climate change, secondary aerosol formation, and aerosol aging. Conventional understanding considers deliquescence of nanosized hygroscopic aerosol particles a nearly instantaneous solid to liquid phase transition. However, the nanoscale dynamics of water condensation and aerosol particle dissolution prior to and during deliquescence remain obscure due to a lack of high spatial and temporal resolution single particle measurements. Here we use real time in situ transmission electron microscopy (TEM) imaging of individual sodium chloride (NaCl) nanoparticles to demonstrate that water adsorption and aerosol particle dissolution prior to and during deliquescence is a multistep dynamic process. Water condensation and aerosol particle dissolution was investigated for lab generated NaCl aerosols and found to occur in three distinct stages as a function of increasing relative humidity (RH). First, a < 100 nm water layer adsorbed on the NaCl cubes and caused sharp corners to dissolve and truncate. The water layer grew to several hundred nanometers with increasing RH and was rapidly saturated with solute, as evidenced by halting of particle dissolution. Adjacent cube corners displayed second-scale curvature fluctuations with no net particle dissolution or water layer thickness change. We propose that droplet solute concentration fluctuations drove NaCl transport from regions of high local curvature to regions of low curvature. Finally, we observed coexistence of a liquid water droplet and aerosol particle immediately prior to deliquescence. Particles dissolved discretely along single crystallographic directions, separated by few second lag times with no dissolution. This work demonstrates that deliquescence of simple pure salt particles with sizes in the range of 100 nm to several microns is not an instantaneous phase transition and instead involves a range of complex dissolution and water condensation dynamics.

Stable isotope compositions, source apportionment and transformation processes of carbonaceous aerosols in PM10 in the urban city of Hyderabad, India

This study apportions sources of carbonaceous aerosols using isotopic characteristics of total carbon (TC) and elemental carbon (EC) in PM10 aerosols using filter-based CTO-375 method for pre-monsoon (summer), post-monsoon, and winter (2019–2021) over Hyderabad, India. Highest secondary organic carbon, SOC (primary organic carbon, POC) of 13.78 ± 10.25 (7.87 ± 2.48) μg/m3 was during post-monsoon 2020 (2019), while lowest was 8.90 ± 5.55 (4.18 ± 0.92) μg/m3 during pre-monsoon 2021 (post-monsoon 2020), respectively. Average effective carbon ratio (ECR) > 1 indicates dominance of light scattering aerosols during pre-monsoon and post-monsoon. δ13CTC and δ13CEC varied from – 28.1 to – 24.7 ‰ (avg. – 26.5 ± 0.7) and - 32.5 to – 24.6 ‰ (avg. – 27.4 ± 1.1), indicating contribution from C3 plant burning and liquid fuel combustion. Positive value of δ13COC – δ13CEC and heavier δ13CTC, along with gradual enrichment in δ13CTC and δ13CEC from December 2020 to March 2021, suggested photochemical aging of carbonaceous aerosols. Lighter δ13CTC and OC/EC > 4 for all seasons indicates dominance of biomass burning (wood and crop residue burning), photochemical oxidation and secondary organic aerosol (SOA) formation. The tropical study experiences dominance of lighter δ13CEC compared to subtropical, high latitude regions.

Investigation on special reactivity of sulfite as an electron acceptor for the attenuated Fenton reaction and the abatement mechanism

Sulfur(IV) as a ubiquitous substance in the atmosphere and water bodies can be deliberately involved in different redox reactions based on the known ability to donate electrons, but the inhibition effect on the advanced oxidation processes (AOPs) especially the Fenton reaction, which played a vital role in aerosol aging and pollution treatment, still stayed fuzzy. In this work, it was first found that sulfite had an unexpected reactivity to accept electrons from Fe(II) monitored by the chemiluminescence (CL) method to reduce Fe(II) seriously. Dynamics calculation, UV–vis absorption, HPLC, and CL analysis indicated that sulfite anions can be transferred into SO2·- or dimer S2O42- through reacting with Fe(II). The direct consumption of Fe(II) in Fenton reaction only happened by sulfite among other inorganic anions during degrading different organic pollution, and the produced S2O42- showed an overpowering inhibitory ability on hydroxyl radical especially at pH 5.3, both resulting in a strong inhibition effect on the Fenton reaction. In contrast at pH 3.1, the fast depletion of sulfite by H2O2 and decomposition of S2O42- fell off the inhibition effect. Furthermore, abatement experiments showed that the effect of sulfite could be circumvented by using a non-iron-based oxidation system with other metal ions, additionally clarifying the reaction of Fe(II)-sulfite played the primary role in the inhibition. Significantly, this inhibition effect of sulfite on the Fenton reaction was demonstrated to take place both in the natural wastewater and degrading two acids from biomass burning in the atmosphere, identifying the attenuated Fenton reaction in the presence of sulfur(IV) in the environment.

Multi-process atmospheric particle number size distribution over the Bohai Sea: Insights from cruise and onboard unmanned aerial vehicle observations

A better understanding of the particle number size distribution aids to better assess the direct and indirect effects of particles on air quality and climate. In this study, particle number concentrations (PNCs) and size distribution along with chemical components, gaseous pollutants, and meteorological parameters were measured during a cruise campaign over the Bohai Sea. Four distinct periods were identified, showing significant impacts from continental outflows and ocean emissions on the particle number size distributions. Under the strong terrestrial pollution transport period, an obvious increase of PNCs below 1 μm was observed. The significant correlation between black carbon (BC) and PNCs in the size range of 0.35–1.0 μm suggested aging of aerosols during the long-range transport. An invaded dust pollution significantly reduced PNCs below 0.5 μm, while tripled the number concentration of particles larger than 0.5 μm. The ocean moisture facilitated the mixing between dust and secondary aerosols. An intense sea fog event observed during the cruise slightly increased PNCs smaller than 1 μm while decreasing larger ones. The correlations between PNCs below 0.5 μm and BC as well as SO2 demonstrated the impact of shipping activities on the formation of fresh particles. Aerosol vertical profiles in the marine boundary layer were measured by an unmanned aerial vehicle platform. The vertical patterns of particle number size distribution were largely governed by the origins of transported air masses and profiles of wind fields. Observations showed that the particle distribution in the lower marine boundary layer was typically inhomogeneous and rapidly evolving with time, highlighting the importance of strengthening the vertical observations of atmospheric parameters over the ocean.

Evolution of refractory black carbon mixing state in an urban environment

The size distribution and hygroscopicity of the refractory black carbon (rBC) aerosol are critical properties for understanding its impact on human health, the extent to which the particles disperse through the atmosphere, and the effect that the particles have on clouds and the climate system. The hygroscopicity of black carbon is primarily controlled by the degree to which the black carbon cores are coated with other compounds. Here we show new measurements of rBC obtained from a single particle soot photometer at an urban location in Houston, TX, USA during the Department of Energy TRacking Aerosol Convection Interactions ExpeRiment (TRACER) campaign. We classified rBC particles into uncoated, thinly coated and thickly coated, where the latter is defined as the optical coating thickness exceeding 10 nm. To understand how aerosol aging and the prevailing winds interact to affect rBC coatings, a slice of the size distribution with rBC core diameter 143–166 nm is considered. For this slice, the average coating thickness of thickly coated particles was 29 ± 8 nm. The rBC number concentration, the fraction of thinly and thickly coated particles, and the average coating thickness strongly vary with the wind direction. We found that onshore flows are associated with lower number concentrations, more thinly coated particles, and thinner coatings when compared to offshore flows. Diurnal profiles show that the fraction of coated particles increases during daytime, likely due to photochemical aging. The estimated fraction of rBC particles that may activate into cloud droplets at 0.1% and 1% water supersaturation was generally ∼0.6% and ∼9%, respectively. This suggests that substantial further aging is needed to precondition the majority of rBC particles for incorporation into cloud droplets.

Assessment of light-absorbing carbonaceous aerosol origins and properties at the ATOLL site in northern France

Abstract. Understanding the lifecycle of light-absorbing carbonaceous aerosols, from emission to deposition, is critical for assessing their climate impact. This study integrated multi-year aerosol observations from the ATOLL (ATmospheric Observations in liLLe, northern France) platform, with air mass back trajectories and emission inventory as a newly developed “INTERPLAY” (IN-siTu obsERvations, hysPLit, And emission inventorY) approach. Applied to black carbon (BC), the method apportioned source contributions (shipping, vehicular, residential heating, industrial) and studied aerosol aging effects, notably on the brown carbon (BrC) component. Results estimate that, throughout the year, vehicular traffic dominated BC (31 %), followed by shipping (25 %, of which one-third was from canals/rivers) and residential heating (21 %). Comparing INTERPLAY results with the aethalometer model highlights that the “residential sector” BC can be entirely apportioned to BC from wood burning (BCwb), notably in winter, while vehicular traffic corresponds to only about 41 % of BC fossil fuel (BCff) at the ATOLL site, the rest being apportioned to shipping (33 %) and industrial (23 %) emissions. Thus, vehicular traffic and BCff should not be used interchangeably, particularly in regions near intense maritime traffic. Concerning BrC, our analysis confirms a dominant role of residential heating. Focusing on winter, results suggest a considerable decrease in the BrC component only 24 h after emission, with fresh residential emissions being responsible for 72 % of BrC absorption at ATOLL. The results from this study allow for an improved understanding of sources and atmospheric dynamics of light-absorbing carbonaceous aerosols in northern France, being crucial for both source abatement strategies as well as a better assessment of their climate impact.

Differences and similarities in optical properties of coated fractal soot and its surrogates

Atmospheric soot (or black carbon, BC) affects climate through solar light absorption and scattering, which depend strongly on the particle morphology and composition. Initially, soot particles are fractal aggregates of spherules made of elemental carbon (EC), but condensation of atmospheric trace vapors adds non-EC materials and often results in particle compaction. The optical properties of such processed soot differ from those of fractal soot, and the changes are caused both by particle volume increase from coating addition and by restructuring of the EC backbone. In laboratory studies of soot optics, surrogates such as carbon black (CB) and nigrosin are often used in place of flame-generated soot. Our goal was to investigate if compositional and morphological differences between these surrogates and soot may produce different processing rates and optical responses. In our experiments, we generated fractal soot, compact CB, agglomerated CB (via coagulation of compact CB), and spherical nigrosin aerosol particles, subjected them to supersaturated vapor of dioctyl sebacate (DOS) to form a coating layer, and investigated the morphological response of these four particle types to coating addition and removal. Using coated and coated-denuded aerosol particles with known composition and morphology, we quantified the contributions of volume increase and restructuring to light scattering and absorption enhancements. By comparing experimental measurements against different particle optics models we show that it is crucial to account for larger, multiply charged particles present in the mobility-classified aerosol. Producing a disproportionately high contribution to absolute values of optical cross sections, such larger particles also result in lesser optical enhancements due to slower growth by vapor condensation. Scattering increases for all particle types due to the addition of a coating layer, and also due to restructuring for fractal soot (strongly) and agglomerated CB (weakly). Absorption increases only due to coating addition caused by the coating layer for all particle types. We find that simple optical models, such as Mie, are often sufficient to provide reasonable closure with experimental results for bare and coated aerosols, but only after accounting for the contributions from multiply charged particles, both in terms of their stronger optical cross sections and slower condensational growth. We conclude that CB is an appropriate surrogate for soot in aerosol aging studies where the effects of restructuring do not need to be considered and that nigrosin can be used as a general model for light-absorbing aerosols but is not representative of optical properties of soot.

Refined Sea Salt Markers for Coastal Cities Facilitating Quantification of Aerosol Aging and PM2.5 Apportionment.

Sea salt (ss) aerosols in PM2.5 are often quantified through source apportionment by applying sodium (Na+) and chloride (Cl-) as the markers, but both markers can be substantially emitted from anthropogenic sources. In this study, we differentiate ss from nonss (nss) portions of Na+ and Cl- to better apportion PM2.5 in a coastal tropical urban environment. Size-resolved ionic profiles accounting for Cl- depletion of aged ss were applied to 162-day measurements during 2012 and 2018-2019. Results show that the nss (likely anthropogenic) portions, on average, account for 50-80% of total Na+ and Cl- in submicron aerosols (PM1). This corresponds to up to 2.5 μg/m3 of ss in submicron aerosols that can be ∼10 times overestimated if one attributes all Na+ and Cl- in PM1 to ss. Employing the newly speciated ss- and nss-portions of Na+ and Cl- to source apportionment of urban PM2.5 via positive matrix factorization uncovers a new source of transported anthropogenic emissions during the southwest monsoon, contributing to 12-15% of PM2.5. This increases anthropogenic PM2.5 by ≥19% and reduces ss-related PM2.5 by >30%. In addition to demonstrating Cl- depletion (aging) in submicron aerosols and quantifying ssNa+, nssNa+, ssCl-, as well as nssCl- therein, the refined PM2.5 apportionment resolves new insights on PM2.5 of anthropogenic origins in urban environments, useful to facilitate policy making.

Insights Into Formation and Aging of Secondary Organic Aerosol From Oxidation Flow Reactors: A Review

Insights Into Formation and Aging of Secondary Organic Aerosol From Oxidation Flow Reactors: A Review

Optical properties and radiative forcing of carbonaceous aerosols in a valley city under persistent high temperature

Carbonaceous aerosols were collected in the valley city of Baoji city in Northern China in August 2022. The light absorption characteristics and influencing factors of black carbon (BC) and brown carbon (BrC) were analyzed, and their radiative forcing was estimated. The results showed that the light absorption of secondary brown carbon [AbsBrC,sec (370)] was 7.5 ± 2.4 Mm−1, which was 2.5 times that of primary brown carbon [AbsBrC,pri (370), 3.0 ± 1.2 Mm−1]. During the study period, the absorption Ångström exponent (AAE) of aerosol was 1.6, indicating that there was obvious secondary aerosol formation or carbonaceous aerosol aging in the valley city of Baoji. Except for secondary BrC (BrCsec), the light absorption coefficient (Abs) and mass absorption efficiency (MAE) of BC and primary BrC (BrCpri) during the persistent high temperature period (PHT) were higher than those during the normal temperature period (NT) and the precipitation period (PP), which indicated that the light absorption capacity of black carbon and primary brown carbon increased, while the light absorption capacity of secondary brown carbon decreased under persistent high temperature period. Secondary aerosols sulfide (SO42−), nitrate (NO3−) and secondary organic carbon (SOC) are important factors for promoting the light absorption enhancemen of BC and BrCpri and photobleaching of BrCsec during persistent high temperature period. The Principal Component Analysis-Multiple Linear Regression (PCA-MLR) model showed that traffic emissions was the most important source of pollution in Baoji City. Based on this, the secondary source accelerates the aging of BC and BrC, causing changes in light absorption. During PHT, the radiative forcing of BC and BrCpri were enhanced, while the radiative forcing of BrCsec was weakened, but the positive radiative forcing generated by them may aggravate the high-temperature disaster.

Atmospheric aerosol chemistry and source apportionment of PM10 using stable carbon isotopes and PMF modelling during fireworks over Hyderabad, southern India

This study examined the influence of fireworks on atmospheric aerosols over the Southern Indian city of Hyderabad during festival of Diwali using mass closure, stable carbon isotopes and the EPA-PMF model. Identification of chemical species in day and night time aerosol samples for 2019 and 2020 Diwali weeks showed increased concentrations of NH4+, NO3−, SO42−, K+, organic carbon (OC), Ba, Pb and Li, which were considered as tracers for fireworks. PM10 source apportionment was done using inorganic (trace elements, major ions) and carbonaceous (organic and elemental carbon; OC & EC) constituents, along with stable isotopic compositions of TC and EC. K+/Na+ ∼1 and K+nss/OC > 0.5 indicated contribution from fireworks. High NO3−, NH4+, Na+, Cl− and SO42− suggested the presence of deliquescent salts NaCl, NH4NO3 and (NH4)2SO4. TAE/TCE >1 suggested H+ exclusion, indicating possible presence of H2SO4 and NH4HSO4 in the aerosols. Ba, Pb, Sb, Sr and Fe increased by 305 (87), 12 (11), 12 (3), 3 (2) and 3 (4) times on Diwali nights, compared to pre-Diwali of 2019 (2020), and are considered as metallic tracers of fireworks. δ13CTC and δ13CEC in aerosols closely resembled that of diesel and C3 plant burning emissions, with meagre contribution from firecrackers during Diwali period. The δ13CEC was relatively depleted than δ13CTC and δ13COC. For both years, δ13COC-EC (δ13COC - δ13CEC) were positive, suggesting photochemical aging of aerosols during long-range transport, while for pre-Diwali 2019 and post-Diwali 2020, δ13COC-EC were negative with high OC/EC ratio, implying secondary organic aerosols formation. High toluene during Diwali week contributed to fresh SOA formation, which reacted with precursor 12C, leading to 13C depletions. Eight-factored EPA-PMF source apportionment indicated highest contribution from residue/waste burning, followed by marine/dust soil and fireworks, while least was contributed from solid fuel/coal combustion.

Role of Hydroperoxyl Radicals in Heterogeneous Oxidation of Oxygenated Organic Aerosols.

Heterogeneous oxidative aging of organic aerosols (OA) occurs ubiquitously in the atmosphere, initiated by oxidants, such as the hydroxyl radicals (•OH). Hydroperoxyl radicals (HO2•) are also an important oxidant in the troposphere, and its gas-phase chemistry has been well studied. However, the role of HO2• in heterogeneous OA oxidation remains elusive. Here, we carry out •OH-initiated heterogeneous oxidation of several OA model systems under different HO2• conditions in a flow tube reactor and characterize the molecular oxidation products using a suite of mass spectrometry instrumentation. By using hydrogen-deuterium exchange (HDX) with thermal desorption iodide-adduct chemical ionization mass spectrometry, we provide direct observation of organic hydroperoxide (ROOH) formation from heterogeneous HO2• and peroxy radicals (RO2•) reactions for the first time. The ROOH may contribute substantially to the oxidation products, varied with the parent OA chemical structure. Furthermore, by regulating RO2• reaction pathways, HO2• also greatly influence the overall composition of the oxidized OA. Last, we suggest that the RO2• + HO2• reactions readily occur at the OA particle interface rather than in the particle bulk. These findings provide new mechanistic insights into the heterogeneous OA oxidation chemistry and help fill the critical knowledge gap in understanding atmospheric OA oxidative aging.

Study of secondary organic aerosol formation and aging using ambient air in an oxidation flow reactor during high pollution events over Delhi

Secondary aerosols constitute a significant fraction of atmospheric aerosols, yet our understanding of their formation mechanism and fate is very limited. In this work, the secondary organic aerosol (SOA) formation and aging of ambient air of Delhi are studied using a potential aerosol mass (PAM) reactor, an oxidation flow reactor (OFR), coupled with aerosol chemical speciation monitor (ACSM), proton transfer reaction time of flight mass spectrometer (PTR-ToF-MS), and scanning mobility particle sizer with counter (SMPS + C). The setup mimics atmospheric aging of up to several days with the generation of OH radicals. Variations in primary volatile organic compounds (VOCs) and oxygenated volatile organic compounds (OVOCs) as a function of photochemical age were investigated. Primary VOCs such as benzene, toluene, xylene, trimethyl benzene, etc. decrease and OVOCs like formic acid, formaldehyde, acetone, ethanol, etc. increase substantially upon oxidation in OFR. The highest organic aerosol (OA) enhancement was observed for the 4.2 equivalent photochemical days of aging i.e., 1.84 times the ambient concentration, and net OA loss was observed at very high OH exposure, typically after 8.4 days of photochemical aging due to heterogeneous oxidation followed by fragmentation/evaporation. In ambient air, OA enhancement is highest during nighttime due to the high concentrations of precursor VOCs in the atmosphere. SMPS + C results demonstrated substantial new particle formation upon aging and decrement in preexisting aerosol mass. This is the first experimental study conducting an in-situ evaluation of potential SOA mass generated from the ambient aerosols in India.

Pollution Characteristics，Sources，and Secondary Generation of Organic Acids in PM2.5 in Zhengzhou

Organic acids in atmospheric particulate matter are widely involved in various physical and chemical reactions in the atmosphere and contribute greatly to the formation of secondary organic aerosols and haze pollutions. Therefore， the concentration distribution characteristics， sources， and secondary formation of organic acids in particulate matter are of great significance for further investigation of organic aerosols and their secondary transformation. Fine particulate matter （PM2.5） samples were collected in Zhengzhou， and three types of organic acids， including dicarboxylic acids， fatty acids， and resin acids， were analyzed to explore their species distribution， seasonal variations， source contribution， and secondary generation. Malonic acid （di-C3） and succinate acid （di-C4） were the most abundant in the identified dicarboxylic acids， which showed obvious seasonal variations in the order of summer &gt; autumn &gt; winter &gt; spring. Fatty acids had the highest concentration in winter and the lowest concentration in spring， showing obvious bimodal advantages， with the most abundant compounds being palmitic acid and stearic acid （C18）. Principal component analysis and multiple linear regression （MLR） were used to analyze the source of organic acids in PM2.5 in Zhengzhou； the results showed that 35% of the organic acids came from combustion and traffic sources， 24% from cooking sources， 23% from secondary formation， and 17% from natural sources. The ratios of the selected marker species （i.e.， di-C3 / di-C4， F/M， and C18：1 / C18） were used as tracers for the secondary formation of the organic aerosol and its aging process. The results showed that the photochemical reaction was intense in summer， and the proportion of organic aerosol aging or secondary production was high， whereas the photochemical reaction was weak in winter， and the aging degree of organic aerosol was low. Correlation analysis and MLR were used in combination to quantify the relative contribution of gas-phase oxidation and liquid-phase oxidation to dicarboxylic acid formation， and the results showed that gas-phase oxidation played a dominant role in the sampling period （accounting for 58%）， especially in summer （61%）.

Review of in vitro studies evaluating respiratory toxicity of aerosols: impact of cell types, chemical composition, and atmospheric processing.

In recent decades, several cell-based and acellular methods have been developed to evaluate ambient particulate matter (PM) toxicity. Although cell-based methods provide a more comprehensive assessment of PM toxicity, their results are difficult to comprehend due to the diversity in cellular endpoints, cell types, and assays and the interference of PM chemical components with some of the assays' techniques. In this review, we attempt to clarify some of these issues. We first discuss the morphological and immunological differences among various macrophage and epithelial cells, belonging to the respiratory systems of human and murine species, used in the in vitro studies evaluating PM toxicity. Then, we review the current state of knowledge on the role of different PM chemical components and the relevance of atmospheric processing and aging of aerosols in the respiratory toxicity of PM. Our review demonstrates the need to adopt more physiologically relevant cellular models such as epithelial (or endothelial) cells instead of macrophages for oxidative stress measurement. We suggest limiting macrophages for investigating other cellular responses (e.g., phagocytosis, inflammation, and DNA damage). Unlike monocultures (of macrophages and epithelial cells), which are generally used to study the direct effects of PM on a given cell type, the use of co-culture systems should be encouraged to investigate a more comprehensive effect of PM in the presence of other cells. Our review has identified two major groups of toxic PM chemical species from the existing literature, i.e., metals (Fe, Cu, Mn, Cr, Ni, and Zn) and organic compounds (PAHs, ketones, aliphatic and chlorinated hydrocarbons, and quinones). However, the relative toxicities of these species are still a matter of debate. Finally, the results of the existing studies investigating the effect of aging on PM toxicity are ambiguous, with varying results due to different cell types, different aging conditions, and the presence/absence of specific oxidants. More systematic studies are necessary to understand the role of different SOA precursors, interactions between different PM components, and aging conditions in the overall toxicity of PM. We anticipate that our review will guide future investigations by helping researchers choose appropriate cell models, resulting in a more meaningful interpretation of cell-based assays and thus ultimately leading to a better understanding of the health effects of PM exposure.

Molecular composition of fresh and aged aerosols from residential wood combustion and gasoline car with modern emission mitigation technology.

Emissions from road traffic and residential heating contribute to urban air pollution. Advances in emission reduction technologies may alter the composition of emissions and affect their fate during atmospheric processing. Here, emissions of a gasoline car and a wood stove, both equipped with modern emission mitigation technology, were photochemically aged in an oxidation flow reactor to the equivalent of one to five days of photochemical aging. Fresh and aged exhausts were analyzed by ultrahigh resolution mass spectrometry. The gasoline car equipped with a three-way catalyst and a gasoline particle filter emitted minor primary fine particulate matter (PM2.5), but aging led to formation of particulate low-volatile, oxygenated and highly nitrogen-containing compounds, formed from volatile organic compounds (VOCs) and gases incl. NOx, SO2, and NH3. Reduction of the particle concentration was also observed for the application of an electrostatic precipitator with residential wood combustion but with no significant effect on the chemical composition of PM2.5. Comparing the effect of short and medium photochemical exposures on PM2.5 of both emission sources indicates a similar trend for formation of new organic compounds with increased carbon oxidation state and nitrogen content. The overall bulk compositions of the studied emission exhausts became more similar by aging, with many newly formed elemental compositions being shared. However, the presence of particulate matter in wood combustion results in differences in the molecular properties of secondary particles, as some compounds were preserved during aging.

Iron content in aerosol particles and its impact on atmospheric chemistry.

Atmospheric aerosol effects on ecological and human health remain uncertain due to their highly complex and evolving nature when suspended in air. Atmospheric chemistry, global climate/oceanic and health exposure models need to incorporate more realistic representations of aerosol particles, especially their bulk and surface chemistry, to account for the evolution in aerosol physicochemical properties with time. (Photo)chemistry driven by iron (Fe) in atmospheric aerosol particles from natural and anthropogenic sources remains limited in these models, particularly under aerosol liquid water conditions. In this feature article, recent advances from our work on Fe (photo)reactivity in multicomponent aerosol systems are highlighted. More specifically, reactions of soluble Fe with aqueous extracts of biomass burning organic aerosols and proxies of humic like substances leading to brown carbon formation are presented. Some of these reactions produced nitrogen-containing gaseous and condensed phase products. For comparison, results from these bulk aqueous phase chemical studies were compared to those from heterogeneous reactions simulating atmospheric aging of Fe-containing reference materials. These materials include Arizona test dust (AZTD) and combustion fly ash particles. Also, dissolution of Fe and other trace elements is presented from simulated human exposure experiments to highlight the impact of aerosol aging on levels of trace metals. The impacts of these chemical reactions on aerosol optical, hygroscopic and morphological properties are also emphasized in light of their importance to aerosol-radiation and aerosol-cloud interactions, in addition to biogeochemical processes at the sea/ocean surface microlayer upon deposition. Future directions for laboratory studies on Fe-driven multiphase chemistry are proposed to advance knowledge and encourage collaborations for efficient utilization of expertise and resources among climate, ocean and health scientific communities.