Wood Burning Emissions Research Articles

Black carbon and particle lung-deposited surface area in residential wood combustion emissions: Effects of an electrostatic precipitator and photochemical aging

Residential wood combustion (RWC) remains a significant global source of particulate matter (PM) emissions with adverse impacts on regional air quality, climate, and human health. The lung-deposited surface area (LDSA) and equivalent black carbon (eBC) concentrations have emerged as important metrics to assess particulate pollution. In this study we estimated combustion phase-dependent emission factors of LDSA for alveolar, tracheobronchial, and head-airway regions of human lungs and explored the relationships between eBC and LDSA in fresh and photochemically aged RWC emissions. Photochemical aging was simulated in an oxidative flow reactor at OH• exposures equivalent to 1.4 or 3.4 days in the atmosphere. Further, the efficiency of a small-scale electrostatic precipitator (ESP) for reducing LDSA and eBC from the wood stove was determined. For fresh emission eBC correlated extremely well with LDSA, but the correlation decreased after aging. Soot-dominated flaming phase showed the highest eBC dependency of LDSA whereas for ignition and char burning phases non-BC particles contributed strongly the LDSA. Deposition to the alveolar region contributed around 60 % of the total lung-deposition. The ESP was found as an effective method to mitigate particulate mass, LDSA, as well as eBC emissions from wood stoves, as they were reduced on average by 72%, 71%, and 69%, respectively. The reduction efficiencies, however, consistently dropped over the span of an experiment, especially for eBC. Further, the ESP was found to increase the sub-30 nm ultrafine particle number emissions, with implications for LDSA. The results of this study can be used for assessing the contribution of RWC to LDSA concentrations in ambient air.

Residential Wood Burning and Vehicle Emissions as Major Sources of Environmentally Persistent Free Radicals in Fairbanks, Alaska.

Environmentally persistent free radicals (EPFRs) play an important role in aerosol effects on air quality and public health, but their atmospheric abundance and sources are poorly understood. We measured EPFRs contained in PM2.5 collected in Fairbanks, Alaska, in winter 2022. We find that EPFR concentrations were enhanced during surface-based inversion and correlate strongly with incomplete combustion markers, including carbon monoxide and elemental carbon (R2 > 0.75). EPFRs exhibit moderately good correlations with PAHs, biomass burning organic aerosols, and potassium (R2 > 0.4). We also observe strong correlations of EPFRs with hydrocarbon-like organic aerosols, Fe and Ti (R2 > 0.6), and single-particle mass spectrometry measurements reveal internal mixing of PAHs, with potassium and iron. These results suggest that residential wood burning and vehicle tailpipes are major sources of EPFRs and nontailpipe emissions, such as brake wear and road dust, may contribute to the stabilization of EPFRs. Exposure to the observed EPFR concentrations (18 ± 12 pmol m-3) would be equivalent to smoking ∼0.4-1 cigarette daily. Very strong correlations (R2 > 0.8) of EPFR with hydroxyl radical formation in surrogate lung fluid indicate that exposure to EPFRs may induce oxidative stress in the human respiratory tract.

Large contribution of in-cloud production of secondary organic aerosol from biomass burning emissions

Organic compounds released from wildfires and residential biomass burning play a crucial role in shaping the composition of the atmosphere. The solubility and subsequent reactions of these compounds in the aqueous phase of clouds and fog remain poorly understood. Nevertheless, these compounds have the potential to become an important source of secondary organic aerosol (SOA). In this study, we simulated the aqueous SOA (aqSOA) from residential wood burning emissions under atmospherically relevant conditions of gas-liquid phase partitioning, using a wetted-wall flow reactor (WFR). We analyzed and quantified the specific compounds present in these emissions at a molecular level and determined their solubility in clouds. Our findings reveal that while 1% of organic compounds are fully water-soluble, 19% exhibit moderate solubility and can partition into the aqueous phase in a thick cloud. Furthermore, it is found that the aqSOA generated in our laboratory experiments has a substantial fraction being attributed to the formation of oligomers in the aqueous phase. We also determined an aqSOA yield of 20% from residential wood combustion, which surpasses current estimates based on gas-phase oxidation. These results indicate that in-cloud chemistry of organic gases emitted from wood burning can serve as an efficient pathway to produce organic aerosols, thus potentially influencing climate and air quality.

Improving residential wood burning emission inventories with the integration of readily available data sources

Residential wood burning (RWB) is the largest anthropogenic source of PM2.5 in many North American and European cities in the winter. The current lack of information on the locations, types, and intensity of use of wood burning appliances limits the ability to accurately assess the exposure of the population to RWB emissions. In this study, we generated a high spatial resolution emission inventory for RWB in the province of Quebec, Canada using a novel data driven approach. The method first combines real estate and socioeconomic census data through machine learning models to estimate ownership rates of fireplaces and wood stoves. These ownership rates are then combined with household survey data (on wood consumption and types of appliances), emission factors and building registry data to generate the emission inventory at a 1Km2 resolution. Our proposed approach was able to capture spatial patterns in RWB appliance ownership and intensity of use, which may be overlooked by using simple urban vs rural or population based spatial proxies. The machine learning models explained 80.3 % and 63 % of the variability in wood stove and fireplace ownership rates with each appliance type exhibiting different spatial trends. Wood stoves were common in rural areas and among lower income households, whereas fireplaces were more common in urban areas. Additionally, we observed large spatial and regional variability in emissions per residence due to differences in wood consumption, appliance ownership rates, and appliance mixes (e.g. conventional vs certified). Our results suggest that using simple spatial proxies based on population, urbanization levels or residence type are not enough to explain the spatial distribution of RWB emissions as they might overlook other factors such as socioeconomic factors or regional heating preferences. Finally, our spatially distributed emissions were strongly correlated (r = 0.86) with the increase in PM2.5 concentrations during peak-RWB hours on winter weekends at 42 reference stations across the province of Quebec.

Assessing the Oxidative Potential of Outdoor PM2.5 in Wintertime Fairbanks, Alaska.

The oxidative potential (OP) of outdoor PM2.5 in wintertime Fairbanks, Alaska, is investigated and compared to those in wintertime Atlanta and Los Angeles. Approximately 40 filter samples collected in January-February 2022 at a Fairbanks residential site were analyzed for OP utilizing dithiothreitol-depletion (OPDTT) and hydroxyl-generation (OPOH) assays. The study-average PM2.5 mass concentration was 12.8 μg/m3, with a 1 h average maximum of 89.0 μg/m3. Regression analysis, correlations with source tracers, and contrast between cold and warmer events indicated that OPDTT was mainly sensitive to copper, elemental carbon, and organic aerosol from residential wood burning, and OPOH to iron and organic aerosol from vehicles. Despite low photochemically-driven oxidation rates, the water-soluble fraction of OPDTT was unusually high at 77%, mainly from wood burning emissions. In contrast to other locations, the Fairbanks average PM2.5 mass concentration was higher than Atlanta and Los Angeles, whereas OPDTT in Fairbanks and Atlanta were similar, and Los Angeles had the highest OPDTT and OPOH. Site differences were observed in OP when normalized by both the volume of air sampled and the particle mass concentration, corresponding to exposure and the intrinsic health-related properties of PM2.5, respectively. The sensitivity of OP assays to specific aerosol components and sources can provide insights beyond the PM2.5 mass concentration when assessing air quality.

A novel measurement system for unattended, in situ characterization of carbonaceous aerosols

Abstract. Carbonaceous aerosol is a relevant constituent of the atmosphere in terms of climate and health impacts. Nevertheless, measuring this component poses many challenges. There is currently no simple and sensitive commercial technique that can reliably capture its totality in an unattended manner, with minimal user intervention, for extended periods of time. To address this issue we have developed the fast thermal carbon totalizator (FATCAT). Our system captures an aerosol sample on a rigid metallic filter and subsequently analyses it by rapidly heating the filter directly, through induction, to a temperature around 800 ∘C. The carbon in the filter is oxidized and quantified as CO2 in order to establish the total carbon (TC) content of the sample. The metallic filter is robust, which solves filter displacement or leakage problems, and does not require a frequent replacement like other measurement techniques. The limit of detection of our system using the 3σ criterion is TC =0.19 µg-C (micrograms of carbon). This translates to an average ambient concentration of TC =0.32 µg-C m−3 and TC =0.16 µg-C m−3 for sampling interval of 1 or 2 h respectively using a sampling flow rate of 10 L min−1. We present a series of measurements using a controlled, well-defined propane flame aerosol as well as wood-burning emissions using two different wood-burning stoves. Furthermore, we complement these measurements by coating the particles with secondary organic matter by means of an oxidation flow reactor. Our device shows a good correlation (correlation coefficient, R2>0.99) with well-established techniques, like mass measurements by means of a tapered element oscillating microbalance and TC measurements by means of thermal–optical transmittance analysis. Furthermore, the homogeneous fast-heating of the filter produces fast thermograms. This is a new feature that, to our knowledge, is exclusive of our system. The fast thermograms contain information regarding the volatility and refractoriness of the sample without imposing an artificial fraction separation like other measurement methods. Different aerosol components, like wood-burning emissions, soot from the propane flame and secondary organic matter, create diverse identifiable patterns.

Contamination Status, Environmental Factor and Risk Assessment of Polychlorinated Biphenyls and Hexachlorobutadiene in Greenhouse and Open-Field Agricultural Soils across China.

With the popularization and high-intensity utilization of greenhouse cultivation for crops growth, the pollution of greenhouse soils has been of concern. Therefore, a national-scale survey was conducted to investigate the contamination status, sources, influence factors and the risks of polychlorinated biphenyls (PCBs) and hexachlorobutadiene (HCBD) in greenhouse and nearby open-field soils. Contents of PCBs ranged from <LOD to 673.78 ng/g (mean: 77.38 ng/g) in greenhouse soils, and <LOD to 552.53 ng/g (mean: 61.90 ng/g) in open-field soils. HCBD was detected in all greenhouse soils with content ranging from 0.85 to 24.18 ng/g (mean: 8.33 ng/g), and a range of <LOD-20.19 ng/g (mean: 6.39 ng/g) in open-field soils. The sources of PCBs were the disposal of electrical equipment, domestic coal, wood burning emissions, etc. Levels of PCBs and HCBD were not correlated with the soil properties but positively correlated with Pseudomonas as the PCBs-degrader in open-field soils. Although the higher values of mean contents were found in greenhouses, the health risks of ΣPCBs in open-field soils were higher than in greenhouse soils due to the higher percentages of high-toxicity PCBs, especially the carcinogenic risks to children (>10-6). This study provided a full insight on the contamination status and risks of PCBs and HCBD when guiding greenhouse agriculture activities.

Molecular compositions and sources of organic aerosols at a rural site on the Guanzhong Plain, Northwest China: The importance of biomass burning

The concentration of PM2.5 has considerably reduced in recent years, but remains relatively high in China. In particular, the increasing contribution of organic compounds to PM2.5 generates popular pressure for further reductions, resulting in an urgent need to study organic aerosol (OA). To investigate the molecular composition and source contribution of OA in the rural area of the Guanzhong Plain, Northwest China, PM2.5 samples were collected during 3–23 August 2016 and 5–20 January 2017 and studied for more than 100 organic tracer compounds. The mean concentration of total measured organic compounds is 662 ± 296 ng/m3 in summer and 3258 ± 1925 ng/m3 in winter. Levoglucosan is the most abundant single compound found throughout the sampling period, which is a crucial tracer for biomass burning emissions, preliminary suggesting that biomass burning is an essential source of OA. In summer, organic compounds such as lipid compounds, sugar compounds, and polycyclic aromatic hydrocarbons (PAHs), more come from higher plants, wood burning, vehicle exhausts, plastic waste, and other direct emission sources. Oxygenated PAHs (OPAHs), nitrophenols, and phthalic acids more come from the atmosphere through the oxidation reaction of aromatic precursors, especially photochemical oxidation. However, in winter, most of the increases in concentrations of organic compounds are attributed to biomass burning. The analysis of a haze event (14–19 January 2017) during the winter sampling period shows that the increases in the concentration of organic compounds are unaccompanied by strong secondary formation under lower relative humidity (49.1% ± 13.5%). The main reason for the growth of OA in this haze event is the accumulation of primary OA (POA). The source apportionment by the positive matrix factorization (PMF) model shows that biomass burning (37.1%) is the primary source of OA in the rural regions of the Guanzhong Plain, especially in winter (40.6%). The contribution of secondary formation decreases from 26.0% in summer to 16.9% in winter, and the contribution of fossil fuel emissions is comparable across both seasons.

Emission of volatile organic compounds from residential biomass burning and their rapid chemical transformations

Biomass combustion releases a complex array of Volatile Organic Compounds (VOCs) that pose significant challenges to air quality and human health. Although biomass burning has been extensively studied at ecosystem levels, understanding the atmospheric transformation and impact on air quality of emissions in urban environments remains challenging due to complex sources and burning materials. In this study, we investigate the VOC emission rates and atmospheric chemical processing of predominantly wood burning emissions in a small urban centre in Greece. Ioannina is situated in a valley within the Dinaric Alps and experiences intense atmospheric pollution accumulation during winter due to its topography and high wood burning activity. During pollution event days, the ambient mixing ratios of key VOC species were found to be similar to those reported for major urban centres worldwide. Positive matrix factorisation (PMF) analysis revealed that biomass burning was the dominant emission source (>50 %), representing two thirds of OH reactivity, which indicates a highly reactive atmospheric mixture. Calculated OH reactivity ranges from 5 s−1 to an unprecedented 278 s−1, and averages at 93 ± 66 s−1 at 9 PM, indicating the presence of exceptionally reactive VOCs. The highly pronounced photochemical formation of organic acids coincided with the formation of ozone, highlighting the significance of secondary formation of pollutants in poorly ventilated urban areas. Our findings underscore the pressing need to transition from wood burning to environmentally friendly sources of energy in poorly ventilated urban areas, in order to improve air quality and safeguard public health.

Assessment of entrainment of key PAHs emanating from major combustion sources into the ambient air

Increasing health problems owing to air pollution is the major cause of concern in the present time, especially in regions with exceptionally high particulate matter (PM) namely Indo-Gangetic Plains (IGP). In the ambient PM, polycyclic aromatic hydrocarbons (PAHs) have been reported to be carcinogenic in nature and its dominant sources are diesel emissions, coal combustion, agricultural waste burning, wood, and cow-dung cake burning. The chemical characteristics of particulate-bound PAHs from all the mentioned sources, their intercomparison, and entrainment into the atmosphere have been assessed in this study. High-molecular weight (HMW) PAHs fraction is highest in emissions from coal combustion (∼95%), followed by agricultural waste burning (83%), wood burning (83%) and cow-dung cake (77%) combustion. Among all the PAH compounds, benzo (b,j) fluoranthene (B[bj]F) was found to be predominant (highest in wood combustion ∼20.3%) in all source samples except exhaust from diesel and bio-diesel engine installed with diesel oxidation catalyst (DOC). Dominant PAH compounds contributing to the carcinogenic potential (CP) are benzo (a) pyrene (B[a]P), dibenzo (a,h) anthracene (D[ah]A), benzo (b,j) fluoranthene (B[bj]F), benzo (a) anthracene (B[a]A) and indeno (1,2,3-c,d) pyrene (IP). Wood combustion (CP = 1.4 ± 0.8) emission is observed to be the most carcinogenic followed by coal combustion (0.8 ± 0.2), diesel exhaust emission (0.4 ± 0.3), cow-dung cake burning (0.2), and agricultural waste burning (0.2 ± 0.1). Further, the range of various diagnostic ratios for each of the source samples has been reported that can be utilized in future studies for more comprehensive source apportionment.

Between Ordinary Harm and Deviance: Evaluating the UK’s Regulatory Regime For Controlling Air Pollution From Wood Burning Stoves

Abstract Particulate matter (PM) in air pollution causes illness, injury and premature death by infiltrating essential organs. Wood burning stoves are a primary source of PM in the United Kingdom, where domestic wood burning emissions have tripled over the last decade. This article adopts a constructivist lens to examine the regulatory regime controlling these pollutants. Combining analysis of ‘expert’ interviews, responses to Freedom of Information requests and government records exempting appliances from Smoke Control Area rules, it illustrates how efforts at controlling ‘smoke’ in the past have become instrumental in encouraging the production of PM from stoves in the present. In doing so, this article demonstrates the utility of research sensitive to processes underpinning the (non)construction of environmental issues as deviant and suggests a lens through which ordinary harms can be better understood.

High-Resolution Emissions from Wood Burning in Norway—The Effect of Cabin Emissions

Emissions from wood burning for heating in secondary homes or cabins is an important part in the development of high-resolution emissions in specific areas. Norway is used as case study as 20% of the national wood consumption for heating occurs in cabins. Our study first shows a method to estimate emissions from cabins based on traffic data to derive cabin occupancy, which combined with heating need allows for the spatial and temporal distribution of emissions. The combination of residential (RWC) and cabin wood combustion (CWC) emissions shows large spatial and temporal differences, and a temporally “cabin population” can in areas be orders of magnitude larger than the registered population. While RWC emissions have been steadily reduced, CWC have kept relatively constant or even increased, which results in an increase in the cabin share to total heating emissions up to 25–35%. When comparing with regional emission inventories, our study shows that the gradient between rural and urban areas is not well-represented in regional inventories, which resembles a population-based distribution and does not allocate emissions in cabin municipalities. CWC emissions may become an increasing environmental concern as higher densification trends in mountain areas are observed.

Long-term trends in particulate matter from wood burning in the United Kingdom: Dependence on weather and social factors

Particulate matter from wood burning emissions (Cwood) was quantified at five locations in the United Kingdom (UK), comprising three rural and two urban sites between 2009 and 2021. The aethalometer method was used. Mean winter Cwood concentrations ranged from 0.26 μg m−3 (in rural Scotland) to 1.30 μg m−3 (London), which represented on average 4% (in rural environments) and 5% (urban) of PM10 concentrations; and 8% of PM2.5. Concentrations were greatest in the evenings in winter months, with larger evening concentrations in the weekends at the urban sites. Random-forest (RF) machine learning regression models were used to reconstruct Cwood concentrations using both meteorological and temporal explanatory variables at each site. The partial dependency plots indicated that temperature and wind speed were the meteorological variables explaining the greatest variability in Cwood, with larger concentrations during cold and calm conditions. Peaks of Cwood concentrations took place during and after events that are celebrated with bonfires. These were Guy Fawkes events in the urban areas and on New Year's Day at the rural sites; the later probably related to long-range transport. Time series were built using the RF. Having removed weather influences, long-term trends of Cwood were estimated using the Theil Sen method. Trends for 2015–2021 were downward at three of the locations (London, Glasgow and rural Scotland), with rates ranging from −5.5% year−1 to −2.5% year−1. The replacement of old fireplaces with lower emission wood stoves might explain the decrease in Cwood especially at the urban sites The two rural sites in England observed positive trends for the same period but this was not statistically significant.

Linking Switzerland's PM&amp;lt;sub&amp;gt;10&amp;lt;/sub&amp;gt; and PM&amp;lt;sub&amp;gt;2.5&amp;lt;/sub&amp;gt; oxidative potential (OP) with emission sources

Abstract. Particulate matter (PM) is the air pollutant that causes the greatest deleterious health effects across the world, so PM is routinely monitored within air quality networks, usually in respect to PM mass or number in different size fractions. However, such measurements do not provide information on the biological toxicity of PM. Oxidative potential (OP) is a complementary metric that aims to classify PM in respect to its oxidising ability in the lungs and is being increasingly reported due to its assumed relevance concerning human health. Between June 2018 and May 2019, an intensive filter-based PM sampling campaign was conducted across Switzerland in five locations, which involved the quantification of a large number of PM constituents and the OP for both PM10 and PM2.5. OP was quantified by three assays: ascorbic acid (AA), dithiothreitol (DTT), and dichlorofluorescein (DCFH). OPv (OP by air volume) was found to be variable over time and space: Bern-Bollwerk, an urban-traffic sampling site, had the greatest levels of OPv among the Swiss sites (especially when considering OPvAA), with more rural locations such as Payerne experiencing a lower OPv. However, urban-background and suburban sites experienced a significant OPv enhancement, as did the rural Magadino-Cadenazzo site during wintertime because of high levels of wood smoke. The mean OP ranges for the sampling period were 0.4–4.1 nmolmin-1m-3, 0.6–3.0 nmolmin-1m-3, and 0.3–0.7 nmol H2O2 m−3 for OPvAA, OPvDTT, and OPvDCFH, respectively. A source allocation method using positive matrix factorisation (PMF) models indicated that although all PM10 and PM2.5 sources that were identified contributed to OPv, the anthropogenic road traffic and wood combustion sources had the greatest OPm potency (OP per PM mass) on average. A dimensionality reduction procedure coupled to multiple linear regression modelling consistently identified a handful of metals usually associated with non-exhaust emissions, namely copper, zinc, iron, tin, antimony, manganese, and cadmium, as well as three specific wood-burning-sourced organic tracers – levoglucosan, mannosan, and galactosan (or their metal substitutes: rubidium and potassium), as the most important PM components to explain and predict OPv. The combination of a metal and a wood-burning-specific tracer led to the best-performing linear models to explain OPv. Interestingly, within the non-exhaust and wood combustion emission groups, the exact choice of component was not critical; the models simply required a variable representing the emission source or process to be present. This analysis strongly suggests that anthropogenic and locally emitting road traffic and wood burning sources should be prioritised, targeted, and controlled to gain the most efficacious decrease in OPv and presumably biological harm reductions in Switzerland.

Fragment ion–functional group relationships in organic aerosols using aerosol mass spectrometry and mid-infrared spectroscopy

Abstract. Aerosol mass spectrometry (AMS) and mid-infrared spectroscopy (MIR) are two analytical methods for characterizing the chemical composition of organic matter (OM). While AMS provides high-temporal-resolution bulk measurements, the extensive fragmentation during the electron ionization makes the characterization of OM components limited. The analysis of aerosols collected on polytetrafluoroethylene (PTFE) filters using MIR, on the other hand, provides functional group information with reduced sample alteration but results in a relatively low temporal resolution. In this work, we compared and combined MIR and AMS measurements for several environmental chamber experiments of combustion-related aerosols to achieve a better understanding of the AMS spectra and the OM chemical evolution with aging. Fresh emissions of wood and coal burning were injected into an environmental simulation chamber and aged with hydroxyl and nitrate radicals. A high-resolution time-of-flight AMS measured the bulk chemical composition of fine OM. Fine aerosols were also sampled on PTFE filters before and after aging for the offline MIR analysis. After comparing AMS and MIR bulk measurements, we used multivariate statistics to identify the functional groups associated the most with the AMS OM for different aerosol sources and oxidants. We also identified the key fragment ions resulting from molecules containing each functional group for the complex OM generated from biomass and fossil fuel combustion. Finally, we developed a statistical model that enables the estimation of the high-time-resolution functional group composition of OM using collocated AMS and MIR measurements. AMS spectra can be used to interpolate the functional group measurements by MIR using this approach. The latter allows us to better understand the evolution of OM during the aging process.

Impacts of severe residential wood burning on atmospheric processing, water-soluble organic aerosol and light absorption, in an inland city of Southeastern Europe

This study examines the concentrations and characteristics of carbonaceous aerosols (including saccharides) and inorganic species measured by PM2.5 filter sampling and a multi-wavelength Aethalometer during two campaigns in a mountainous, medium-sized, Greek city (Ioannina). The first campaign was conducted in summer and used as a baseline of low concentrations, while the second took place in winter under intensive residential wood burning (RWB) emissions. Very high winter-mean OC concentrations (26.0 μg m−3) were observed, associated with an OC/EC ratio of 9.9, and mean BCwb and PM2.5 levels of 4.5 μg m−3 and 57.5 μg m−3, respectively. Simultaneously, record-high levoglucosan (Lev) concentrations (mean: 6.0 μg m−3; max: 15.9 μg m−3) were measured, revealing a severely biomass burning (BB)-laden environment. The water-soluble OC component (WSOC) accounted for 56 ± 9% of OC in winter, exhibiting high correlations (R2 = 0.93–0.97) with BB tracers (nss-K+, BCwb, Lev), nitrate and light absorption, potentially indicating the formation of water-soluble brown carbon (BrC) from fast oxidation processes. The examination of diagnostic ratios involving BB tracers indicated the prevalence of hardwood burning, while the mean Lev/OC ratio (22%) was remarkably higher than literature values. Applying a mono-tracer method based on levoglucosan, we estimated very high BB contributions to OC (∼92%), EC (∼64%) and WSOC (∼87%) during winter. On the contrary, low levels were registered during summer for all carbonaceous components, with winter/summer ratios of 4–5 for PM2.5 and BC, 10 for OC, 30 for BCwb and ∼1100 for levoglucosan. The absence of local BB sources in summer, combined with the photochemical processing and aging of regional organic aerosols, resulted in higher WSOC/OC fractions (64 ± 13%). The results indicate highly soluble fine carbonaceous aerosol fraction year-round, which when considered alongside the extreme concentration levels in winter can have important implications for short- and long-term health effects.

Polycyclic Aromatic Hydrocarbons in the Marine Atmosphere from the Western Pacific to the Southern Ocean: Spatial Variability, Gas/Particle Partitioning, and Source Apportionment.

The spatial variability of polycyclic aromatic hydrocarbons (PAHs) in the marine atmosphere contributes to the understanding of the global sources, fate, and impact of this contaminant. Few studies conducted to measure PAHs in the oceanic atmosphere have covered a large scale, especially in the Southern Ocean. In this study, high-volume air samples were taken along a cross-section from China to Antarctica and analyzed for gaseous and particulate PAHs. The data revealed the spatial distribution, gas-particle partitioning, and source contributions of PAHs in the Pacific, Indian, and Southern Oceans. The median concentration (gaseous + particulate) of ∑24PAHs was 3900 pg/m3 in the Pacific Ocean, 2000 pg/m3 in the Indian Ocean, and 1200 pg/m3 in the Southern Ocean. A clear latitudinal gradient was observed for airborne PAHs from the western Pacific to the Southern Ocean. Back trajectories (BTs) analysis showed that air masses predominantly originated from populated land had significantly higher concentrations of PAHs than those from the oceans or Antarctic continents/islands. The air mass origins and temperature have significant influences on the gas-particle partitioning of PAHs. Source analysis by positive matrix factorization (PMF) showed that the highest contribution to PAHs was from coal combustion emissions (52%), followed by engine combustion emissions (27%) and wood combustion emissions (21%). A higher contribution of PAHs from wood combustion was found in the eastern coastal region of Australia. In contrast, engine combustion emissions primarily influenced the sites in Southeast Asia.

Modelling aerosol molecular markers in a 3D air quality model: Focus on anthropogenic organic markers

We developed and implemented in the 3D air quality model CHIMERE the formation of several key anthropogenic aerosol markers including one primary anthropogenic marker (levoglucosan) and 4 secondary anthropogenic markers (nitrophenols, nitroguaiacols, methylnitrocatechols and phthalic acid). Modelled concentrations have been compared to measurements performed at 12 locations in France for levoglucosan in winter 2014–15, and at a sub-urban station in the Paris region over the whole year 2015 for secondary molecular markers. While a good estimation of levoglucosan concentrations by the model has been obtained for a few sites, a strong underestimation was simulated for most of the stations especially for western locations due to a probable underestimation of residential wood burning emissions. The simulated ratio between wood burning organic matter and particulate phase levoglucosan is constant only at high OM values (>10 μg m−3) indicating that using marker contribution ratio may be valid only under certain conditions. Concentrations of secondary markers were well reproduced by the model for nitrophenols and nitroguaiacols but were underestimated for methylnitrocatechols and phthalic acid highlighting missing formation pathways and/or precursor emissions. By comparing modelled to measured Gas/Particle Partitioning (GPP) of markers, the simulated partitioning of Semi-Volatile Organic Compounds (SVOCs) was evaluated. Except for nitroguaiacols and nitrophenols when ideality was assumed, the GPP for all the markers was underestimated and mainly driven by the hydrophilic partitioning. SVOCs GPP, and more generally of all SVOC contributing to the formation of SOA, could therefore be significantly underestimated by air quality models, especially when only the partitioning on the organic phase is considered. Our results show that marker modelling can give insights on some processes (such as precursor emissions or missing mechanisms) involved in SOA formation and could prove especially useful to evaluate the GPP in 3D air quality models.

Seasonal variability of nitroaromatic compounds in ambient aerosols: Mass size distribution, possible sources and contribution to water-soluble brown carbon light absorption

Nitroaromatic compounds (NACs) as important constituents of atmospheric humic-like substances (HULIS) and brown carbon (BrC) affect the Earth's climate and pose a serious environmental hazard. We investigated seasonal size-segregated NACs in aerosol samples from the urban background environment in Ljubljana, Slovenia. Total concentrations of twenty NACs in PM15.6 were on average from 0.51 ng m−3 (summer) to 109 ng m−3 (winter), and contributed the most to submicron aerosols (more than 74%). Besides 4-nitrocatechol (4NC) as the prevailing species, methylnitrocatechols (MNCs) and nitrophenols (NPs), we reported on some very rarely mentioned, but also on five novel NACs (i.e., 3H4NBA: 3-hydroxy-4-nitrobenzoic acid, 3MeO4NP: 3-methoxy-4-nitrophenol, 4Et5NC: 4-ethyl-5-nitrocatechol, 3Et5NC: 3-ethyl-5-nitrocatechol and 3MeO5NC: 3-methoxy-5-nitrocatechol). Concentrations of 3MeO5NC, 4Et5NC and 3Et5NC were enhanced during cold seasons, contributing up to 11% to total NAC in winter. In cold season, NAC size distributions were characterized with the peaks in the broader size range of 0.305–1.01 μm (accumulation mode), with 4NC and alkyl-nitrocatechols (∑(M/Et)NC) as the most abundant, followed by 4-nitrosyringol, nitrophenols and nitroguaiacols. In spring, a pronounced peak of ∑(M/Et)NC was observed in the accumulation mode (0.305–0.56 μm) as well as in the coarse one. A strong correlation of all NACs with ∑(M/Et)NC and levoglucosan indicates that primary emissions of wood burning were the most important source of NACs, but their secondary formation (e.g., aqueous-phase at higher ambient RH) in cold season could also be a significant one. In warmer season, NACs may be mostly derived from traffic-related aromatic VOCs. The contribution of NACs to the light absorption of the aqueous extracts was up to 10-times higher (contribution to Abs365 up to 31%) than their mass contributions to WSOC (up to 3%) of corresponding size-segregated aerosols, confirming that most of the identified NACs are strong BrC chromophores.

An evaluation of the photochemical air quality modeling using CMAQ in the industrial area of Quintero-Puchuncavi-Concon, Chile

The air pollution has impacted for years the population and the ecosystem in the industrial area located in Quintero, Puchuncavi, and Concon counties, the coastal area of Central Chile. In this study, we used the WRF-SMOKE-CMAQ model system to evaluate the photochemical modeling of PM10, PM2.5, and O3. The industrial and the residential wood combustion sources were the main contributors of particulate matter, sulfur dioxide and volatile organic compounds. The small diurnal temperature cycle, the high relative humidity and the low wind speed profiles exposed the meteorological condition of the coastal lows during the period of analysis. The daily average concentrations for PM10 and PM2.5 ranged from 24.03 to 50.10 μg/m3 and 15.60–21.95 μg/m3 for observed registries; meanwhile, the simulated results were in the range of 22.71–40.62 μg/m3 and 5.49–17.29 μg/m3, respectively. The omission of missing sources in the emission inventory and the default values in the boundary condition could be one of the reasons on the underprediction obtained. The best performance for O3 occurred in the Quintero and Sur stations, located near industrial sources with high NOx and VOC emissions. In the industrial complex, PM10 and PM2.5 concentrations were 10–30 μg/m3 lower when the industrial emissions were shut down and a negligible difference was observed when the residential wood combustion emissions were not considered. Future air quality modeling must be performed in the same region for other periods like the Summer season. Also, the emission inventory from all sources needs to be accurate with more accurate temporal profiles.