Residential Wood Combustion 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.

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.

The contribution of residential wood combustion to the PM2.5 concentrations in the Helsinki metropolitan area

Abstract. This article has investigated the contribution of residential wood combustion (RWC) to the fine particulate matter (PM2.5) concentrations in the Helsinki metropolitan area (HMA) for 6 years, from 2009 to 2014. We have used the PM2.5 concentrations measured at eight air quality measurement stations. The dispersion of emissions on an urban scale was evaluated with multiple-source Gaussian dispersion models, UDM-FMI (urban dispersion model of the Finnish Meteorological Institute) and CAR-FMI (Contaminants in the Air from a Road model of the Finnish Meteorological Institute), and on a regional scale using the chemical transport model SILAM (System for Integrated modeLling of Atmospheric coMposition). The overall agreement of the predicted concentrations with measurements of PM2.5 was good or fairly good for all stations and years; e.g. at the permanent residential station the daily average values of the index of agreement ranged from 0.69 to 0.81, and the fractional bias values ranged from −0.08 to 0.11, for the considered 6 years. Both the measured and predicted daily averaged concentrations showed increasing trends towards the lower-temperature values. The highest predicted annual averaged concentrations in the region occurred in the vicinity of major roads and streets and in the suburban residential areas to the northwest, north, and northeast of the city centre. The average concentrations of PM2.5 attributed to RWC in winter were up to 10- or 15-fold, compared to the corresponding concentrations in summer. During the considered 6-yearly period, the spatially highest predicted fractions of RWC of the annual PM2.5 concentrations ranged from 12 % to 14 %. In winter, the corresponding contributions ranged from 16 % to 21 %. The RWC contribution was higher than the corresponding urban vehicular traffic contribution at all the residential stations during all years. The study has highlighted new research needs for the future, in particular (i) the modelling of the RWC emissions that would be explicitly based on the actual ambient temperatures and (ii) the modelling of the impacts of the most important holiday periods on the emissions from RWC.

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.

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.

Spatial distribution of residential wood combustion emissions in the Nordic countries: How well national inventories represent local emissions?

Residential wood combustion (RWC) is a major source of air pollutants in the Nordic and many other countries. The emissions of the pollutants have been estimated with inventories on several scopes, e.g. local and national. An important aspect of the inventories is the spatial distribution of the emissions, as it has an effect on health impact assessments. In this study, we present a novel residential wood combustion emission inventory for the Nordic countries based on national inventories and new gridding of the emissions. We compare the emissions of the Nordic inventory, and especially their spatial distribution, to local assessments and European level TNO-newRWC-inventory to assess the spatial proxies used. Common proxies used in the national inventories in the Nordic countries were building data on locations and primary heating methods and questionnaire-based wood use estimates for appliances or primary heating methods. Chimney sweeper register data was identified as good proxy data, but such data may not be available in an applicable format. Comparisons of national inventories to local assessments showed the possibility to achieve similar spatial distributions through nation-wide methods as local ones. However, this won't guarantee that the emissions are similar. Comparison to the TNO-newRWC-inventory revealed the importance of how differences between urban and rural residential wood combustion are handled. The comparison also highlighted the importance of local characteristics of residential wood combustion in the spatial distribution of emissions.

Perinatal health impacts of air pollution mitigation policies: applying g formula to preterm birth in Temuco/Padre Las Casas, Chile

BACKGROUND AND AIM: Wood burning is a primary energy source for heating but constitutes a significant source of PM2.5 emissions and is linked to adverse health outcomes, including preterm birth (PTB). There is little evidence on the expected benefits from air pollution mitigation plans with respect to perinatal outcomes, particularly those aimed at decreasing residential wood-burning emissions. We estimated the magnitude of reduction in prevalence and number of PTB cases associated with compliance with air quality guidelines and specific interventions to reduce fine particulate matter in Temuco/Padre Las Casas, Chile, an area heavily affected by wood burning from residential heating. METHODS: A parametric G-computation approach was applied to quantify the relationship between PM2.5 and time to PTB. We relied on a retrospective cohort of all live births between 2009-2015 from a public hospital in Temuco (n=15,516). We simulated the effects of four scenarios to reduce PM2.5 as compared to “business as usual” (no intervention): compliance with i) WHO guidelines; ii) Chilean limit values; reductions associated with iii) a wood heater replacement program and iv) gradual prohibition of less efficient stoves/heaters. RESULTS:Women were exposed to high levels of air pollution in each trimester of pregnancy (30 µg/m3 in each trimester); 10% of births were PTB. Both prevalence and number of cases of PTB decreased with each intervention scenario, with larger decreases associated with compliance to national limits and international guidelines. For gradual prohibition of less efficient stoves, expected prevalence of PTB was 8% compared to 5.7% associated with compliance with Chilean limits, which represented 225 (95% CI -395, -56) and 544 (95% CI -897, -190) fewer cases of PTB compared to business as usual. CONCLUSIONS:We found large potential benefits for prevalence and number of PTB cases associated with the mitigation strategies, with larger reductions for norm compliance compared to specific wood-burning proposed. KEYWORDS: air pollution, mitigation strategies, adverse birth outcomes, G methods

In situ identification of aerosol types in Athens, Greece, based on long-term optical and on online chemical characterization

Absorption Ångström Exponent (AAE) and Scattering Ångström Exponent (SAE) values, derived from aethalometer and nephelometer measurements during a period of 3 years at an urban background site in Athens, are combined for the first aerosol type classification using in situ measurements in the eastern Mediterranean. In addition, single scattering albedo (SSA) and its wavelength dependence (dSSA), as well as the chemical composition of fine aerosols and precursor gases from collocated measurements, are utilized to provide further insights on the optical-chemical characterization and related sources of seven identified aerosol types. Urban aerosols are mostly characterized as Black Carbon (BC)-dominated (76.3%), representing a background atmosphere where fossil-fuel combustion is dominant throughout the year, while 14.3% of the cases correspond to the mixed Brown Carbon (BrC)-BC type, with a higher frequency in winter. The BrC type is associated with the highest scattering and absorption coefficients during winter nights, representing the impact from residential wood-burning emissions. Dust mixed with urban pollution (1.2%) and large particles mixed with BC (5.3%) have a higher frequency in spring. Furthermore, aging processes and BC coating with organic and inorganic species with weak spectral absorption (AAE<1) account for 2.2%, with a differentiation between small and large particles. dSSA is recognized as a useful parameter for aerosol characterization, since fine aerosols are associated with negative dSSA values. The identified aerosol types are examined on a seasonal, monthly, hourly basis and by potential source areas, as well as in comparison with fine-aerosol chemical composition and apportioned organic aerosol source contributions, in an attempt to explore the linkage between optical, physical and chemical aerosol properties. Chemical analysis indicates high organic fraction (60–68%) for the BrC and BrC/BC, 20–30% larger compared to other types. The results are essential for parametrization in chemical transport models and for reducing the uncertainty in the assessment of aerosol radiative effects.

Photochemical transformation of residential wood combustion emissions: dependence of organic aerosol composition on OH exposure

Abstract. Residential wood combustion (RWC) emits large amounts of gaseous and particulate organic aerosol (OA). In the atmosphere, the emission is transformed via oxidative reactions, which are under daylight conditions driven mainly by hydroxyl radicals (OH). This continuing oxidative ageing produces secondary OA and may change the health- and climate-related properties of the emission. However, it is not well known how the composition of RWC-originated OA changes as the function of OH exposure. In this work, emissions from two modern residential logwood combustion appliances were photochemically aged in an oxidation flow reactor (OFR) with various OH exposure levels, reaching up to 6×1011 s cm−3 (equivalent to 1 week in the atmosphere). Gaseous organic compounds were analysed by proton transfer reaction time-of-flight mass spectrometry (PTR-ToF-MS), while particulate OA was analysed online by a high-resolution soot particle aerosol mass spectrometer (SP-HR-ToF-AMS) and offline by in situ derivatization thermal desorption–gas chromatography–time-of-flight mass spectrometry (IDTD-GC-ToF-MS). Photochemical reactions increased the mass of particulate organic carbon by a factor of 1.3–3.9. The increase in mass took place during the first atmospheric equivalent day of ageing, after which the enhancement was independent of the extent of photochemical exposure. However, ageing increased the oxidation state of the particulate OA linearly throughout the assessed range, with ΔH:C/ΔO:C slopes between −0.17 and −0.49 in van Krevelen space. Ageing led to an increase in acidic fragmentation products in both phases, as measured by the IDTD-GC-ToF-MS for the particulate and PTR-ToF-MS for the gaseous phase. For the gaseous organic compounds, the formation of small carbonylic compounds combined with the rapid degradation of primary volatile organic compounds such as aromatic compounds led to a continuous increase in both the O : C and H : C ratios. Overall, the share of polycyclic aromatic compounds (PACs) in particles degraded rapidly during ageing, although some oxygen-substituted PACs, most notably naphthaldehydic acid, increased, in particular during relatively short exposures. Similarly, the concentrations of particulate nitrophenols rose extensively during the first atmospheric equivalent day. During continuous photochemical ageing, the dominant transformation mechanisms shifted from the initial gas-phase functionalization/condensation to the transformation of the particulate OA by further oxidation reactions and fragmentation. The observed continuous transformation of OA composition throughout a broad range of OH exposures indicates that the entire atmospheric lifetime of the emission needs to be explored to fully assess the potential climate and health effects of RWC emissions.

Six-year source apportionment of submicron organic aerosols from near-continuous highly time-resolved measurements at SIRTA (Paris area, France)

Abstract. Organic aerosol (OA) particles are recognized as key factors influencing air quality and climate change. However, highly time-resolved long-term characterizations of their composition and sources in ambient air are still very limited due to challenging continuous observations. Here, we present an analysis of long-term variability of submicron OA using the combination of an aerosol chemical speciation monitor (ACSM) and a multiwavelength Aethalometer from November 2011 to March 2018 at a peri-urban background site of the Paris region (France). Source apportionment of OA was achieved via partially constrained positive matrix factorization (PMF) using the multilinear engine (ME-2). Two primary OA (POA) and two oxygenated OA (OOA) factors were identified and quantified over the entire studied period. POA factors were designated as hydrocarbon-like OA (HOA) and biomass burning OA (BBOA). The latter factor presented a significant seasonality with higher concentrations in winter with significant monthly contributions to OA (18 %–33 %) due to enhanced residential wood burning emissions. HOA mainly originated from traffic emissions but was also influenced by biomass burning in cold periods. OOA factors were distinguished between their less- and more-oxidized fractions (LO-OOA and MO-OOA, respectively). These factors presented distinct seasonal patterns, associated with different atmospheric formation pathways. A pronounced increase in LO-OOA concentrations and contributions (50 %–66 %) was observed in summer, which may be mainly explained by secondary OA (SOA) formation processes involving biogenic gaseous precursors. Conversely, high concentrations and OA contributions (32 %–62 %) of MO-OOA during winter and spring seasons were partly associated with anthropogenic emissions and/or long-range transport from northeastern Europe. The contribution of the different OA factors as a function of OA mass loading highlighted the dominant roles of POA during pollution episodes in fall and winter and of SOA for highest springtime and summertime OA concentrations. Finally, long-term trend analyses indicated a decreasing feature (of about −175 ng m−3 yr−1) for MO-OOA, very limited or insignificant decreasing trends for primary anthropogenic carbonaceous aerosols (BBOA and HOA, along with the fossil-fuel and biomass-burning black carbon components) and no statistically significant trend for LO-OOA over the 6-year investigated period.

Long-term brown carbon spectral characteristics in a Mediterranean city (Athens)

This study analyses 4-years of continuous 7-λ Aethalometer (AE-33) measurements in an urban-background environment of Athens, to resolve the spectral absorption coefficients (babs) for black carbon (BC) and brown carbon (BrC). An important BrC contribution (23.7 ± 11.6%) to the total babs at 370 nm is estimated for the period May 2015–April 2019, characterized by a remarkable seasonality with winter maximum (33.5 ± 13.6%) and summer minimum (18.5 ± 8.1%), while at longer wavelengths the BrC contribution is significantly reduced (6.8 ± 3.6% at 660 nm). The wavelength dependence of the total babs gives an annual-mean AAE370-880 of 1.31, with higher values in winter night-time. The BrC absorption and its contribution to babs presents a large increase reaching up to 39.1 ± 13.6% during winter nights (370 nm), suggesting residential wood burning (RWB) emissions as a dominant source for BrC. This is supported by strong correlations of the BrC absorption with OC, EC, the fragment ion m/z 60 derived from ACSM and PMF-analyzed organic fractions related to biomass burning (e.g. BBOA). In contrast, BrC absorption decreases significantly during daytime as well as in the warm period, reaching to a minimum during the early-afternoon hours in all seasons due to photo-chemical degradation. Estimated secondary BrC absorption is practically evident only during winter night-time, implying the fast oxidation of BrC species from RWB emissions. Changes in mixing-layer height do not significantly affect the BrC absorption in winter, while they play a major role in summer.

Long-term variability, source apportionment and spectral properties of black carbon at an urban background site in Athens, Greece

This study aims to delineate the characteristics of Black Carbon (BC) in the atmosphere over Athens, Greece, using 4-year (May 2015–April 2019) Aethalometer (AE-33) measurements. The average BC concentration is 1.9 ± 2.5 μg m−3 (ranging from 0.1 to 32.7 μg m−3; hourly values), with a well-defined seasonality from 1.3 ± 1.1 μg m−3 in summer to 3.0 ± 4.0 μg m−3 in winter. Pronounced morning and evening/night peaks are found in the BC concentrations in winter, while during the rest of the seasons, this diurnal cycle appears to flatten out, with the exception of the morning traffic peak. On an annual basis, the biomass-burning fraction (BB%) of BC accounts for 22 ± 12%, while the fossil-fuel combustion (BCff) component (traffic emissions and domestic heating) dominates during summer (83%) and in the morning hours. BCwb exhibits higher contribution in winter (32%), especially during the night hours (39%). BC levels are effectively reduced by precipitation, while they significantly build-up for wind speeds <3 m s−1 and mixing-layer height (MLH) < 500 m. Normalizing the BC diurnal course by the MLH variations on a seasonal basis reveals that the residential wood-burning emissions are mostly responsible for the large BC increase during winter nights, whereas the low BC levels during daytime in the warm season are mainly attributed to dilution into a deeper MLH. BCwb is highly correlated with other BB tracers during winter nights (e.g. levoglucosan, non-sea-salt-K+, m/z 60 fragment), as well as with the fine fraction (PM2.5) OC and EC. The Delta-C, which represents the spectral dependence of BC as the absorption difference between 370 and 880 nm, is analyzed for the first time in Athens. It exhibits a pronounced seasonality with maximum values in winter night-time, and it appears as a valid qualitative marker for wood combustion.

Production of particulate brown carbon during atmospheric aging of residential wood-burning emissions

Abstract. We investigate the optical properties of light-absorbing organic carbon (brown carbon) from domestic wood combustion as a function of simulated atmospheric aging. At shorter wavelengths (370–470 nm), light absorption by brown carbon from primary organic aerosol (POA) and secondary organic aerosol (SOA) formed during aging was around 10 % and 20 %, respectively, of the total aerosol absorption (brown carbon plus black carbon). The mass absorption cross section (MAC) determined for black carbon (BC, 13.7 m2 g−1 at 370 nm, with geometric standard deviation GSD =1.1) was consistent with that recommended by Bond et al. (2006). The corresponding MAC of POA (5.5 m2 g−1; GSD =1.2) was higher than that of SOA (2.4 m2 g−1; GSD =1.3) at 370 nm. However, SOA presents a substantial mass fraction, with a measured average SOA ∕ POA mass ratio after aging of ∼5 and therefore contributes significantly to the overall light absorption, highlighting the importance of wood-combustion SOA as a source of atmospheric brown carbon. The wavelength dependence of POA and SOA light absorption between 370 and 660 nm is well described with absorption Ångström exponents of 4.6 and 5.6, respectively. UV-visible absorbance measurements of water and methanol-extracted OA were also performed, showing that the majority of the light-absorbing OA is water insoluble even after aging.

2014 residential wood combustion survey: Results overview and spatial allocation of emissions estimates

Through the use of monitoring, modeling, and emission inventories, the Oregon Department of Environmental Quality (DEQ) has identified residential wood combustion (RWC) as a significant source of air pollution in Oregon. Detailed emission inventories provide the best source of information to inform pollution reduction strategies. In order to refine and improve state and local RWC emission inventories, DEQ contracted with the Portland State University Survey Research Lab to perform a telephone survey on RWC in the Portland metro area. The goal of the project was to 1) quantify these emissions by type and location, and 2) to spatially allocate these emissions to US Census blocks in the study area and other parts of the state. Results, based on 1061 residences surveyed, showed that 4.3% of respondents burned wood for primary heating and 17.8% burned wood for secondary (backup heating or aesthetics) purposes. Primary burners burned four times more wood on average per device than secondary burners. As such, even though there were fewer primary burners they burned 51% of the total wood fuel combusted. The breakdown of estimated emissions of particulate matter 2.5 μm or less (PM2.5) from primary and secondary burners is nearly even, with 46.5% of emissions coming from primary burning and 53.5% of emissions coming from secondary burning. Uncertified woodstoves and inserts are the source of just over half (50.5%) the emissions in the Survey area, followed by emissions from certified woodstoves and inserts (26.3%), fireplaces (21.5%), pellet stoves (0.9%), and fire-log burning (0.8%). Survey results for burning activity and housing type showed good correlation, and were mapped to US Census housing data (units in structure) for block-groups. The Survey results also showed differences in burning behavior between urban/suburban and rural areas. This distinction coupled with housing types provided a method of spatial allocation for RWC activity and emissions that could be a useful tool for other states and regions.

Observations of biomass burning tracers in PM2.5 at two megacities in North China during 2014 APEC summit

To evaluate the effectiveness of biomass burning control measures on PM2.5 reduction, day- and nighttime PM2.5 samples were collected at two urban sites in North China, one in Beijing (BJ) and the other in Shijiazhuang (SJZ), during the 2014 Asia-Pacific Economic Cooperation (APEC) summit. Typical biomass burning aerosol tracers including levoglucosan (LG), Mannosan (MN), and water-soluble potassium (K+), together with other water-soluble ions and carbonaceous species were determined. The levels of biomass burning tracers dropped dramatically during the APEC period when open biomass burning activities were well controlled in North China, yet they increased sharply to even higher levels during the post-APEC period. Distinct linear regression relationships between LG and MN were found with lower LG/MN ratios from periods with much reduced open biomass burning activities. This was likely resulted from the reduced open crop residues burning and increased residential wood burning emissions, as was also supported by the simultaneous decrease in K+/LG ratio. The positive matrix factorization and air quality model simulation analyses suggested that PM2.5 concentration produced from biomass burning sources was reduced by 22% at BJ and 46% at SJZ during the APEC period compared to pre-APEC period, although they increased to higher levels after APEC mainly due to increased residential biomass burning emissions in winter heating season. Biomass burning was also found to be the most important contributor to carbonaceous species that might cause significant light extinction in this region. This study not only suggested implementing biomass burning controls measures were helpful to reduce PM2.5 in North China, but also pointed out both open crop residues burning and indoor biomass burning activities could make substantial contributions to PM2.5 and its major components in urban areas in North China.

Characterization of gas-phase organics using proton transfer reaction time-of-flight mass spectrometry: fresh and aged residential wood combustion emissions

Abstract. Organic gases emitted during the flaming phase of residential wood combustion are characterized individually and by functionality using proton transfer reaction time-of-flight mass spectrometry. The evolution of the organic gases is monitored during photochemical aging. Primary gaseous emissions are dominated by oxygenated species (e.g., acetic acid, acetaldehyde, phenol and methanol), many of which have deleterious health effects and play an important role in atmospheric processes such as secondary organic aerosol formation and ozone production. Residential wood combustion emissions differ considerably from open biomass burning in both absolute magnitude and relative composition. Ratios of acetonitrile, a potential biomass burning marker, to CO are considerably lower ( ∼ 0.09 pptv ppbv−1) than those observed in air masses influenced by open burning ( ∼ 1–2 pptv ppbv−1), which may make differentiation from background levels difficult, even in regions heavily impacted by residential wood burning. A considerable amount of formic acid forms during aging ( ∼ 200–600 mg kg−1 at an OH exposure of (4.5–5.5) × 107 molec cm−3 h), indicating residential wood combustion can be an important local source for this acid, the quantities of which are currently underestimated in models. Phthalic anhydride, a naphthalene oxidation product, is also formed in considerable quantities with aging ( ∼ 55–75 mg kg−1 at an OH exposure of (4.5–5.5) × 107 molec cm−3 h). Although total NMOG emissions vary by up to a factor of ∼ 9 between burns, SOA formation potential does not scale with total NMOG emissions and is similar in all experiments. This study is the first thorough characterization of both primary and aged organic gases from residential wood combustion and provides a benchmark for comparison of emissions generated under different burn parameters.

Untargeted Identification of Wood Type-Specific Markers in Particulate Matter from Wood Combustion.

Residential wood combustion emissions are one of the major global sources of particulate and gaseous organic pollutants. However, the detailed chemical compositions of these emissions are poorly characterized due to their highly complex molecular compositions, nonideal combustion conditions, and sample preparation steps. In this study, the particulate organic emissions from a masonry heater using three types of wood logs, namely, beech, birch, and spruce, were chemically characterized using thermal desorption in situ derivatization coupled to a GCxGC-ToF/MS system. Untargeted data analyses were performed using the comprehensive measurements. Univariate and multivariate chemometric tools, such as analysis of variance (ANOVA), principal component analysis (PCA), and ANOVA simultaneous component analysis (ASCA), were used to reduce the data to highly significant and wood type-specific features. This study reveals substances not previously considered in the literature as meaningful markers for differentiation among wood types.

Particulate emissions from residential wood combustion in Europe – revised estimates and an evaluation

Abstract. Currently residential wood combustion (RWC) is increasing in Europe because of rising fossil fuel prices but also due to climate change mitigation policies. However, especially in small-scale applications, RWC may cause high emissions of particulate matter (PM). Recently we have developed a new high-resolution (7 × 7 km) anthropogenic carbonaceous aerosol emission inventory for Europe. The inventory indicated that about half of the total PM2.5 emission in Europe is carbonaceous aerosol and identified RWC as the largest organic aerosol source in Europe. The inventory was partly based on national reported PM emissions. Use of this organic aerosol inventory as input for two chemical transport models (CTMs), PMCAMx and EMEP MSC-W, revealed major underestimations of organic aerosol in winter time, especially for regions dominated by RWC. Interestingly, this was not universal but appeared to differ by country. In the present study we constructed a revised bottom-up emission inventory for RWC accounting for the semivolatile components of the emissions. The revised RWC emissions are higher than those in the previous inventory by a factor of 2–3 but with substantial inter-country variation. The new emission inventory served as input for the CTMs and a substantially improved agreement between measured and predicted organic aerosol was found. The revised RWC inventory improves the model-calculated organic aerosol significantly. Comparisons to Scandinavian source apportionment studies also indicate substantial improvements in the modelled wood-burning component of organic aerosol. This suggests that primary organic aerosol emission inventories need to be revised to include the semivolatile organic aerosol that is formed almost instantaneously due to dilution and cooling of the flue gas or exhaust. Since RWC is a key source of fine PM in Europe, a major revision of the emission estimates as proposed here is likely to influence source–receptor matrices and modelled source apportionment. Since usage of biofuels in small combustion units is a globally significant source, the findings presented here are also relevant for regions outside of Europe.

Effects of Residential Wood-Burning Emissions during Winter Months in a Northern San Diego County Location

Ambient particulate matter (PM10 and PM2.5) and carbon monoxide (CO) due to domestic wood burning during the winter and summer months in the city of Escondido were investigated. The data collected from January 2000 to December 2010 from San Diego Air Pollution Control District's (SDAPCD's) collection station in Escondido were analyzed by both non-paired student's t-tests and Mann-Whitney U tests (significance of 0.05 for both tests). For all three pollutants, the significant differences in levels between the winter and summer months, the significant differences in levels during the days that were celebrated as holidays and normal days, and the significant differences in levels between weekends and weekdays were noted. Additionally, the significant differences in levels between night and daytime, early evening hours and night and during burning and smoldering fires were determined for hourly PM2.5 and CO data. For all emission types, traffic patterns did not match the levels of emissions on weekdays, weekends, evenings, or daytimes. Elemental and organic carbon species taken from PM2.5 data correlated with the original PM2.5 filter data. Results of our analysis suggest that wood burning is a source of PM10, PM2.5, and CO in the area.

Light-absorbing carbon in Europe – measurement and modelling, with a focus on residential wood combustion emissions

Abstract. The atmospheric concentration of elemental carbon (EC) in Europe during the six-year period 2005–2010 has been simulated with the EMEP MSC-W model. The model bias compared to EC measurements was less than 20% for most of the examined sites. The model results suggest that fossil fuel combustion is the dominant source of EC in most of Europe but that there are important contributions also from residential wood burning during the cold seasons and, during certain episodes, also from open biomass burning (wildfires and agricultural fires). The modelled contributions from open biomass fires to ground level concentrations of EC were small at the sites included in the present study, &lt;3% of the long-term average of EC in PM10. The modelling of this EC source is subject to many uncertainties, and it was likely underestimated for some episodes. EC measurements and modelled EC were also compared to optical measurements of black carbon (BC). The relationships between EC and BC (as given by mass absorption cross section, MAC, values) differed widely between the sites, and the correlation between observed EC and BC is sometimes poor, making it difficult to compare results using the two techniques and limiting the comparability of BC measurements to model EC results. A new bottom-up emission inventory for carbonaceous aerosol from residential wood combustion has been applied. For some countries the new inventory has substantially different EC emissions compared to earlier estimates. For northern Europe the most significant changes are much lower emissions in Norway and higher emissions in neighbouring Sweden and Finland. For Norway and Sweden, comparisons to source-apportionment data from winter campaigns indicate that the new inventory may improve model-calculated EC from wood burning. Finally, three different model setups were tested with variable atmospheric lifetimes of EC in order to evaluate the model sensitivity to the assumptions regarding hygroscopicity and atmospheric ageing of EC. The standard ageing scheme leads to a rapid transformation of the emitted hydrophobic EC to hygroscopic particles, and generates similar results when assuming that all EC is aged at the point of emission. Assuming hydrophobic emissions and no ageing leads to higher EC concentrations. For the more remote sites, the observed EC concentration was in between the modelled EC using standard ageing and the scenario treating EC as hydrophobic. This could indicate too-rapid EC ageing in the model in relatively clean parts of the atmosphere.