Biomass Burning Sources Research Articles

Improved simulations of biomass burning aerosol optical properties and lifetimes in the NASA GEOS Model during the ORACLES-I campaign

Abstract. In order to improve aerosol representation in the NASA Goddard Earth Observing System (GEOS) model, we evaluated simulations of the transport and properties of aerosols from southern African biomass burning sources that were observed during the first deployment of the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) field campaign in September 2016. An example case study of 24 September was analyzed in detail, during which aircraft-based in situ and remote sensing observations showed the presence of a multi-layered smoke plume structure with significant vertical variation in single scattering albedo (SSA). Our baseline GEOS simulations were not able to represent the observed SSA variation or the observed organic aerosol-to-black-carbon ratio (OA : BC). Analyzing the simulated smoke age suggests that the higher-altitude, less absorbing smoke plume was younger (∼4 d), while the lower-altitude and more absorbing smoke plume was older (∼7 d). We hypothesize a chemical or microphysical loss process exists to explain the change in aerosol absorption as the smoke plume ages, and we apply a simple loss rate to the model hydrophilic biomass burning OA to simulate this process. We also utilized the ORACLES airborne observations to better constrain the simulation of aerosol optical properties, adjusting the assumed particle size, hygroscopic growth, and absorption. Our final GEOS model simulation with additional OA loss and updated optics showed better performance in simulating aerosol optical depth (AOD) and SSA compared to independent ground- and space-based retrievals for the entire month of September 2016, including the Ozone Monitoring Instrument (OMI) Aerosol Index. In terms of radiative implications of our model adjustments, the final GEOS simulation suggested a decreased atmospheric warming of about 10 % (∼2 W m−2) over the southeastern Atlantic region and above the stratocumulus cloud decks compared to the model baseline simulations. These results improve the representation of the smoke age, transport, and optical properties in Earth system models.

Direct radiative forcing of light-absorbing carbonaceous aerosols in China

China is an important emitter of light-absorbing carbonaceous aerosols (LACs), including black carbon (BC) and brown carbon (BrC). Currently, there are large uncertainties in model-estimated direct radiative forcing (DRF) of LACs, partially due to the poor understanding of the emissions and optical properties of LACs. In this study, we estimated the DRF of LACs over China during the implementation of the Air Pollution Prevention and Control Action Plan (APPCAP) using the global chemical transport model (GEOS-Chem) coupled with the Rapid Radiative Transfer Model of GCMs (RRTMG). We updated the refractive index of BC, includedbiomass burning (BB) sources, biofuel (BF) and coal combustion (CC) sources in the residential sector as BrC emission sources and the optical properties were updated, which were not fully considered in the previous model studies. Our results showed that model could reasonably capture the spatial and temporal variations of LACs in China with the correlation coefficients between model simulated and Aerosol Robotic Network (AERONET) observed daily absorption aerosol optical depth (AAOD) of LACs at 440 nm above 0.63 and the corresponding values of the normalized mean bias within ±30%. The simulated annual mean LACs AAOD at 440 nm in China was 0.016 (0.021) in 2017 (2014) and BrC contributed about 20% (21%). The estimated annual mean clear-sky LACs DRF at the top of the atmosphere in China was 1.02 W m−2 in 2017 and 1.38 W m−2 in 2014, and the contribution of BrC was about 10% and 11%, respectively, which was dominated by the BF sources (46% in 2017 and 44% in 2014) and the BB sources (38% in 2017 and 43% in 2014), with CC sources being low (16% in 2017 and 13% in 2014). The annual mean AAOD and DRF of LACs in China decreased by 0.005 and 0.36 W m−2 from 2014 to 2017, which were largely attributed to the reductions of anthropogenic emissions during the implementation of APPCAP. Our results would improve the understanding of the light absorption capacity and climate effects of LACs in China.

Impacts of open biomass burning in Southeast Asia on atmospheric PM2.5 concentrations over south China from 2009 to 2018

Open biomass burning (BB) frequently occurs in spring over Southeast Asia (SEA). The concentration of fine particulate (PM2.5) produced by BB and its impacts on air quality in downwind aeras exhibit significant interannual variations, which are controlled by emission intensity and meteorological circulation. In this study, a regional air quality model system (RAQMS) was applied to investigate the contributions of BB emissions in SEA to atmospheric PM2.5 concentrations over South China in March (a spring month) during 2009–2018 and their interannual variations. Higher near-surface BB-PM2.5 (refers to the PM2.5 produced by BB in SEA) concentrations and contributions were mainly distributed in the source region and its vicinity, while the higher tropospheric BB-PM2.5 concentrations and contributions were characterized by a long belt extending from BB source regions to Yangtze River Delta (YRD) in South China. Combined with the vertical distribution of BB-PM2.5 on the transported path profile, it indicated that higher BB-PM2.5 concentrations were mainly concentrated in 0∼1500 m above the ground over source regions, while the maximum BB-PM2.5 concentrations in the downwind area were distributed in 1500∼3500 m above the ground. The monthly mean tropospheric BB-PM2.5 concentrations were higher in March 2009, 2010, 2012, and 2013, with evident correlation with interannual variation of BB emissions. Sensitivity experiments suggested that the near-surface and tropospheric BB-PM2.5 concentrations over South China had changed by-48.1%∼190.5% and −48.0%∼213.8%, respectively in March 2009–2018 by fixing BB emissions unchanged at the mean of the 10 years, being greater than the changes caused by meteorological conditions and other affecting factors (∼20%). In addition, the relative contributions of BB emission from various regions in SEA on the mean near-surface and tropospheric BB-PM2.5 concentrations over South China were further identified.

Source apportionment of black carbon using an advanced Aethalometer model in a typical industrial city of China

Black carbon (BC) aerosol can lead to adverse health effects and drive climate change; therefore, the characteristic research and identification of BC sources are essential for lowering emissions. In this study, equivalent black carbon (eBC) measurement was performed using a seven-wavelength Aethalometer (AE33) at an urban site in a typical industrial city (Zibo) of Northern China for the first time. The monitoring was performed from February 2021 to January 2022. The mass absorption cross-section (MAC) of AE33 was optimised using the online elemental carbon (EC) data, and eBC was corrected using the MAC. The corrected annual BC concentration was 1.72 ± 1.18 µg/m3. The diurnal variation of BC depicted a bimodal distribution. Furthermore, the BC concentration on weekends was 18% lower than on weekdays. The diurnal variation and weekend effect reflect the critical contributions of traffic emission to BC concentration. The source apportionment of BC was calculated by a constraining Aethalometer model, which restricted the Ångström exponent using the online potassium ions. The results revealed that BC was not significantly affected by biomass burning (BCbb) in Zibo. The relative contribution of BCbb was higher in winter than in other seasons. The daily morning peak of BC was primarily influenced by traffic sources, whereas the contribution of biomass burning increased after 17:00 in the evening peak. Our findings suggest that it is more important to control fossil fuel sources for BC emission reduction in Zibo, while it is necessary to strengthen the control of biomass combustion sources in winter.

Organic tracers in fine and coarse aerosols at an urban Mediterranean site: contribution of biomass burning and biogenic emissions.

The concentrations of anhydrosugars (levoglucosan, mannosan, and galactosan), polyols (inositol, xylitol, sorbitol, and mannitol), and glucose were measured in PM1 and PM10 samples collected during 1 year at a traffic site in the city of Elche (southeastern Spain). Levoglucosan, mannosan, and galactosan were mainly found in the PM1 fraction since they are mainly emitted from biomass burning (BB). Likewise, inositol, xylitol, and sorbitol were primarily distributed in the fine mode, suggesting a non-negligible contribution from anthropogenic sources (specifically BB) to the levels of these compounds. This was supported by their seasonal variations, with higher concentrations during winter, and their correlations with levoglucosan concentrations. The average contributions of biomass burning and biogenic sources to OC and PM levels were calculated using levoglucosan and mannitol, respectively, as tracers. On average, BB accounted for 12% and 16% of the OC in PM1 and PM10, while the estimated contribution of fungal spores to OC and PM10 levels was 1.2 and 0.8%, respectively. The results of the present study suggest that, at least in the study area, most sugar alcohols are not appropriate tracers of biogenic emissions.

Spatial-temporal Distribution and Source Analysis of Polycyclic Aromatic Hydrocarbons in the Sediments of Poyang Lake

The concentrations, spatial-temporal distribution, and influencing factors of 16 polycyclic aromatic hydrocarbons (PAHs) in the sediments of Poyang Lake were studied, and a quantitative source analysis of PAHs in different areas of the lake was conducted. PAHs were widespread within the sediments. The concentrations of ∑16PAHs in the surface sediments of all sites ranged from 203 to 2 318 μg·kg-1. The concentrations of PAHs in the surface sediments of the lake body were higher than those in the surface sediments of the inlet rivers. The ratio of PAHs in Poyang Lake was 4 rings > 5 rings > 6 rings > 3 rings > 2 rings; the composition of 4-ring PAHs was dominant, and its content accounted for 86.11% of ∑16PAHs. The 2- and 3-ring and some 4-ring PAHs, including Flua and Pyr, were more susceptible to SOM, and the 4 through 6-ring PAHs were more susceptible to ORP and heavy metals and other environmental factors. Spatially, the higher concentration of ∑16PAHs occurred in the area of the lake adjacent to Duchang County and Poyang County, where the terrain was relatively closed, and the water exchange with the surrounding area was less than that in other sections, which was not conducive to the migration, transformation, and degradation of pollutants. In the temporal distribution, the changes in PAHs concentration level and the development of GDP in Jiangxi Province showed high consistency, and the influence of economic development and human activities might have been the main reason for the increasing PAHs concentration level. The main sources of PAHs in surface sediments of Poyang Lake included petroleum pollution and oil and coal and biomass combustion sources, and there were some spatial differences in PAHs sources in different regions. This study can provide a reference for PAHs pollution in surface sediments of Poyang Lake, which is important for the ecological environmental protection and management of Poyang Lake.

Characteristics and Source Analysis of Carbonaceous Aerosols in PM2.5 in Huaxi District, Guiyang

Carbonaceous aerosol, as an important component of atmospheric aerosol, has a significant impact on atmospheric environmental quality, human health, and global climate change. To investigate the characteristics and sources of carbonaceous aerosol in atmospheric fine particulate matter (PM2.5) in Huaxi District of Guiyang, an in-situ observational study was conducted during different seasons in 2020, and the carbonaceous components of PM2.5 were measured using a thermal-optical carbon analyzer (DRI Model 2015). The results of the study showed that the average concentrations of PM2.5, total carbonaceous aerosol (TCA), organic carbon (OC), secondary organic carbon (SOC), and elemental carbon (EC) concentrations during the observation period were (39.7±22.3), (14.1±7.2), (7.6±3.9), (4.4±2.6), and (2.0±1.0) μg·m-3, respectively, and the mean value of OC/EC was (3.9±0.8). ρ(PM2.5), ρ(TCA), ρ(OC), ρ(SOC), and ρ(EC) showed a seasonal variation pattern with the highest in winter [(52.6±28.6), (17.0±9.6), (9.1±5.2), (6.1±3.9), and (2.4±1.2) μg·m-3, respectively] and the lowest in summer [(25.1±7.1), (11.6±3.6), (6.3±1.9), (3.7±1.2), and (1.6±0.6) μg·m-3, respectively]. The seasonal variation in OC/EC showed summer (4.2±0.8) > winter (3.8±0.9) > autumn (3.8±0.5) > spring (3.7±0.9), indicating the presence of SOC generation in all seasons in Huaxi District. SOC showed a significant correlation with OC (R2 =0.9), and the SOC concentration tended to increase with the increase in atmospheric oxidation. OC showed a good correlation with EC in all seasons, with the highest in autumn (R2 =0.9) and lower correlations in the other three seasons (R2 ranged from 0.74 to 0.75), indicating a common source. According to OC/EC ratio range, it was preliminarily determined that carbonaceous aerosol came from vehicle exhaust emissions, coal burning emissions, and biomass combustion emissions. In order to further quantify the contribution of major emission sources to carbonaceous aerosol, the results of this study using PMF to analyze the sources of carbonaceous aerosol showed that the main sources of carbonaceous aerosol in Huaxi District of Guiyang were coal combustion sources (29.3%), motor vehicle emission sources (21.5%), and biomass combustion sources (49.2%).

Tropical tropospheric aerosol sources and chemical composition observed at high altitude in the Bolivian Andes

Abstract. The chemical composition of PM10 and non-overlapping PM2.5 was studied at the summit of Mt. Chacaltaya (5380 m a.s.l., lat. −16.346950°, long. −68.128250°) providing a unique long-term record spanning from December 2011 to March 2020. The chemical composition of aerosol at the Chacaltaya Global Atmosphere Watch (GAW) site is representative of the regional background, seasonally affected by biomass burning practices and by nearby anthropogenic emissions from the metropolitan area of La Paz–El Alto. Concentration levels are clearly influenced by seasons with minima occurring during the wet season (December to March) and maxima occurring during the dry and transition seasons (April to November). Ions, total carbon (EC + OC), and saccharide interquartile ranges for concentrations are 558–1785, 384–1120, and 4.3–25.5 ng m−3 for bulk PM10 and 917–2308, 519–1175, and 3.9–24.1 ng m−3 for PM2.5, respectively, with most of the aerosol seemingly present in the PM2.5 fraction. Such concentrations are overall lower compared to other high-altitude stations around the globe but higher than Amazonian remote sites (except for OC). For PM10, there is dominance of insoluble mineral matter (33 %–56 % of the mass), organic matter (7 %–34 %), and secondary inorganic aerosol (15 %–26 %). Chemical composition profiles were identified for different origins: EC, NO3-, NH4+, glucose, and C2O42- for the nearby urban and rural areas; OC, EC, NO3-, K+, acetate, formate, levoglucosan, and some F− and Br− for biomass burning; MeSO3-, Na+, Mg2+, K+, and Ca2+ for aged marine emissions from the Pacific Ocean; arabitol, mannitol, and glucose for biogenic emissions; Na+, Ca2+, Mg2+, and K+ for soil dust; and SO42-, F−, and some Cl− for volcanism. Regional biomass burning practices influence the soluble fraction of the aerosol between June and November. The organic fraction is present all year round and has both anthropogenic (biomass burning and other combustion sources) and natural (primary and secondary biogenic emissions) origins, with the OC/EC mass ratio being practically constant all year round (10.5 ± 5.7, IQR 8.1–13.3). Peruvian volcanism has dominated the SO42- concentration since 2014, though it presents strong temporal variability due to the intermittence of the sources and seasonal changes in the transport patterns. These measurements represent some of the first long-term observations of aerosol chemical composition at a continental high-altitude site in the tropical Southern Hemisphere.

Chemical composition, sources and formation mechanism of urban PM2.5 in Southwest China: a case study at the beginning of 2023

Abstract. Despite significant improvements in air quality in recent years, the Sichuan Basin (SCB) is still facing frequent haze pollution in winter, and the causes of severe haze formation have not yet been fully investigated. In this study, the chemical components of PM2.5 (i.e., particulate matter with an aerodynamic diameter of less than 2.5 µm) in a typical pollution period at the beginning of 2023 in Chengdu, a megacity in the SCB, were characterized by bulk-chemical and single-particle analysis, and the PM2.5 sources and formation mechanism of pollution were analyzed. The average mass concentration of PM2.5 during the study period was 95.6 ± 28.7 µg m−3. Organic matter (OM) was the most abundant component (35.3 %), followed by nitrate (22.0 %), sulfate (9.2 %) and ammonium (7.8 %). The individual aerosol particles were classified into five categories, i.e., mineral, OM, secondary inorganic aerosol (SIA), soot and fly ash/metal particles, and most of them were in the state of being internally mixed. The entire observation period could be divided into two non-pollution periods (NP-1 and NP-2) and two haze periods (Haze-1 and Haze-2). With the evolution of pollution, the bulk-chemical and single-particle analysis exhibited similar characteristics, suggesting that Haze-1 was mainly caused by pollutants related to fossil fuel combustion, especially local mobile sources, while Haze-2 was triggered by the rapidly increasing secondary pollutants, which mainly came from regional transmission. The PM2.5 sources included dust (8.5 %), biomass burning (3.5 %), coal combustion (15.4 %), industrial processes (6.5 %), vehicular emissions (25.6 %) and secondary sources (40.5 %). Analysis of Weather Research and Forecasting model with Chemistry (WRF-Chem) model results showed that the average contributions of local sources and regional transmission to pollution in Chengdu were the same (50 % vs. 50 %). In addition, the source composition and WRF-Chem simulation results in different periods confirmed our analysis of the formation mechanisms of the two haze events. This study confirms that further significant reductions in PM2.5 in Chengdu are still needed, and more effective policies for local emission reduction or joint prevention and control of regional air pollution will be necessary in the future.

Effects of UAS Rotor Wash on Air Quality Measurements.

Laboratory and field tests examined the potential for unmanned aircraft system (UAS) rotor wash effects on gas and particle measurements from a biomass combustion source. Tests compared simultaneous placement of two sets of CO and CO2 gas sensors and PM2.5 instruments on a UAS body and on a vertical or horizontal extension arm beyond the rotors. For 1 Hz temporal concentration comparisons, correlations of body versus arm placement for the PM2.5 particle sensors yielded R2 = 0.85 and for both gas sensor pairs exceeded R2 of 0.90. Increasing the timestep to 10 s average concentrations throughout the burns improved the R2 value for the PM2.5 to 0.95 from 0.85. Finally, comparison of whole-test average concentrations further increased the correlations between body- and arm-mounted sensors, exceeding R2 of 0.98 for both gases and particle measurements. Evaluation of PM2.5 emission factors with single factor ANOVA analyses showed no significant differences between the values derived from the arm, either vertical or horizontal, and those from the body. These results suggest that rotor wash effects on body- and arm-mounted sensors are minimal in scenarios where short duration, time-averaged concentrations are used to calculate emission factors and whole-area flux values.

Observationally constrained analysis of sulfur cycle in the marine atmosphere with NASA ATom measurements and AeroCom model simulations

Abstract. The atmospheric sulfur cycle plays a key role in air quality, climate, and ecosystems, such as pollution, radiative forcing, new particle formation, and acid rain. In this study, we compare the spatially and temporally resolved measurements from the NASA Atmospheric Tomography (ATom) mission with simulations from five AeroCom III models for four sulfur species (dimethyl sulfide (DMS), sulfur dioxide (SO2), particulate methanesulfonate (MSA), and particulate sulfate (SO4)). We focus on remote regions over the Pacific, Atlantic, and Southern oceans from near the surface to ∼ 12 km altitude range covering all four seasons. In general, the differences among model results can be greater than 1 order of magnitude. Comparing with observations, model-simulated SO2 is generally low, whereas SO4 is generally high. Simulated DMS concentrations near the sea surface exceed observed levels by a factor of 5 in most cases, suggesting potential overestimation of DMS emissions in all models. With GEOS model simulations of tagging emission from anthropogenic, biomass burning, volcanic, and oceanic sources, we find that anthropogenic emissions are the dominant source of sulfate aerosol (40 %–60 % of the total amount) in the ATom measurements at almost all altitudes, followed by volcanic emissions (18 %–32 %) and oceanic sources (16 %–32 %). Similar source contributions can also be derived at broad ocean basins and on monthly scales, indicating the representativeness of ATom measurements for global ocean. Our work presents the first assessment of AeroCom sulfur study using ATom measurements, providing directions for improving sulfate simulations, which remain the largest uncertainty in radiative forcing estimates in aerosol climate models.

Impact of anthropogenic emission control in reducing future PM2.5 concentrations and the related oxidative potential across different regions of China

Affected by both future anthropogenic emissions and climate change, future prediction of PM2.5 and its Oxidative Potential (OP) distribution is a significant challenge, especially in developing countries like China. To overcome this challenge, we estimated historical and future PM2.5 concentrations and associated OP using the Danish Eulerian Hemispheric Model (DEHM) system with meteorological input from WRF weather forecast model. Considering different future socio-economic pathways and emission scenario assumptions, we quantified how the contribution from various anthropogenic emission sectors will change under these scenarios. Results show that compared to the CESM_SSP2–4.5_CLE scenario (based on moderate radiative forcing and Current Legislation Emission), the CESM_SSP1–2.6_MFR scenario (based on sustainability development and Maximum Feasible Reductions) is projected to yield greater environmental and health benefits in the future. Under the CESM_SSP1–2.6_MFR scenario, annual average PM2.5 concentrations (OP) are expected to decrease to 30 μgm−3 (0.8 nmolmin−1m−3) in almost all regions by 2030, which will be 65 % (67 %) lower than that in 2010. From a long-term perspective, it is anticipated that OP in the Fen-Wei Plain region will experience the maximum reduction (82.6 %) from 2010 to 2049. Largely benefiting from the effective control of PM2.5 in the region, it has decreased by 82.1 %. Crucially, once emission reduction measures reach a certain level (in 2040), further reductions become less significant. This study also emphasized the significant role of secondary aerosol formation and biomass-burning sources in influencing OP during both historical and future periods. In different scenarios, the reduction range of OP from 2010 to 2049 is estimated to be between 71 % and 85 % by controlling precursor emissions involved in secondary aerosol formation and emissions from biomass burning. Results indicate that strengthening the control of anthropogenic emissions in various regions are key to achieving air quality targets and safeguarding human health in the future.

Unambiguous Analysis and Systematic Mapping of Oxygenated Aromatic Compounds in Atmospheric Aerosols Using Ultrahigh-Resolution Mass Spectrometry.

Compositional analysis of organic aerosols (OAs) at the molecular level has been a long-standing challenge in field and laboratory studies. In this work, we applied different extraction protocols to aerosol samples collected from the ambient atmosphere and biomass burning sources, followed by Orbitrap mass spectrometric analysis with a soft electrospray ionization source operating in both positive and negative ionization modes. To systematically map the distribution of mono- and dioxygenated aromatic compounds (referred to as aromatic CHO1 and CHO2 formulas) in OA, we developed a unique two-dimensional Kendrick mass defect (2D KMD) framework. Our analysis unveiled a total of (76, 64, 70) aromatic CHO1 formulas and (103, 110, 106) CHO2 formulas, corresponding to samples obtained from ambient air, rice straw burning, and sugarcane leaf burning, respectively. These results reveal a significant number of additional distinct formulas exclusively present in ambient samples, suggesting a significant chemical transformation of OAs in the atmosphere. The analytical approach can be further extended to incorporate multiple layers of 2D KMD, enabling systematic mapping of the unexplored chemical space for complex environmental samples.

Source apportionment of fine and ultrafine particle number concentrations in a major city of the Eastern Mediterranean

Ultrafine particles (UFP) are recognized as an emerging pollutant able to induce serious health effects. However, quantitative information regarding the contributions of UFP sources is generally limited. This study evaluates statistical (k-means clustering) and receptor models (Positive Matrix Factorization - PMF) using particle number size distributions (PNSD), along with chemical speciation data, measured at an urban background supersite in Athens, Greece, aiming to characterize their sources. PNSD measurements (10–487 nm) were performed during three distinct periods (warm, cold, and lockdown cold). Traffic and residential biomass burning (BB) produced high UFP number concentrations (NUFP) in the cold period (+107 % compared to summer), while the lockdown restrictions reduced NUFP (−42 %). The five groups produced by cluster analysis that were common among periods were linked to high- and low-traffic, new particle formation (NPF), urban background and regional aerosols. PMF source apportionment identified 5 and 6 factors during warm and cold periods, respectively, indicating that traffic particles dominated NUFP (64–78 % in all periods), while accumulation-mode particles and volume concentrations were controlled by processed aerosol, and especially in the cold periods by BB emissions. A nucleation factor linked to NPF contributed 7–11 % to NUFP. Comparing the two cold periods (business-as-usual, lockdown), important lockdown reductions (−46 %) were seen for fresh traffic contributions to total number concentration (Ntotal). The impact of the source attributed to NPF also eroded (−41 % for Ntotal). Due to the large reduction (−47 % for Ntotal) observed also for the BB source during the lockdown (reduced wood usage due to a milder winter), the relative contributions of all sources did not change considerably (fractional reductions <7 % for Ntotal). The quantitative results, bolstered by source apportionment combining PNSD and online chemical composition measurements, indicate the potential to constrain UFP levels by regulating traffic and residential emissions, with a large upside for population exposure control.

Economic and Industrial Development SignificantlyContribute to Acidity and Ionic Compositions of Rainwaterin China

To achieve a holistic understanding of the intricate interactions among human activities, atmospheric chemistry, and acid rain in China, a rigorous analysis of rainwater chemistry was made using a dataset comprising 2656 data points from 24 sites. The main cation and anion in the chemical composition of precipitation were Ca2+ and SO42− in China, with an average concentration of 169.9 μeq/L and 135.4 μeq/L, respectively. Acid rain generally occurs in southern cities such as Shenzhen, Guangzhou, Zhuhai, Xiamen, and Chongqing. There were evident regional disparities in acidity and ion concentrations in rainwater, with an increase in acidity and a decrease in ion concentrations from north to south across China. Utilizing positive matrix factorization, the study found that NH4+, SO42−, and NO3− mainly originated from anthropogenic sources such as fossil fuel combustion, vehicle exhaust emissions, agricultural fertilization, and industrial emissions (as reflected by F3 and F4). Ca2+ mainly stems from crustal factors, including industrial dust and natural crust (as represented by F1 and F4). Na+ and Cl− were traceable from marine sources (as reflected by F5), while Mg2+ originated from crust origin (as presented by F1). K+ was mainly derived from a mixed source of crust, marine, and biomass burning (as indicated by F2 and F3). The correlation analyses showed that SO42− and NO3− showed significant correlations with GDP and population. F− was associated with wastewater, which may be linked to the production of brick and tiles from clay with high fluoride contents. The pH was negatively related to industrial wastewater. Long-term analysis of precipitation chemistry in four cities suggested a clear decrease in the proportion of SO42− but a considerable increase in the proportion of NO3− in anions in metropolitans of Shanghai and Chongqing due to the environmental measures that targeted reducing sulfur dioxide (SO2) emissions and increase of vehicles. This showed that pollution control strategies had an impact on precipitation ion concentrations. These results can conclude that economic and industrial growth, which will increase energy consumption, utilization of coal combustion, and a subsequent rise in pollutant emissions, can contribute to the change in the chemical compositions of rainwater and the exacerbation of acid rain.

Contributions of Biomass Burning and Other Sources to Fine Particle Level and Oxidative Potential in Suburban Tokyo, Japan

Contributions of Biomass Burning and Other Sources to Fine Particle Level and Oxidative Potential in Suburban Tokyo, Japan

Aerosol source apportionment uncertainty linked to the choice of input chemical components

For a Positive Matrix Factorization (PMF) aerosol source apportionment (SA) studies there is no standard procedure to select the most appropriate chemical components to be included in the input dataset for a given site typology, nor specific recommendations in this direction. However, these choices are crucial for the final SA outputs not only in terms of number of sources identified but also, and consequently, in the source contributions estimates. In fact, PMF tends to reproduce most of PM mass measured independently and introduced as a total variable in the input data, regardless of the percentage of PM mass which has been chemically characterized, so that the lack of some specific source tracers (e.g. levoglucosan) can potentially affect the results of the whole source apportionment study. The present study elaborates further on the same concept, evaluating quantitatively the impact of lacking specific sources’ tracers on the whole source apportionment, both in terms of identified sources and source contributions. This work aims to provide first recommendations on the most suitable and critical components to be included in PMF analyses in order to reduce PMF output uncertainty as much as possible, and better represent the most commons PM sources observed in many sites in Western countries. To this aim, we performed three sensitivity analyses on three different datasets across EU, including extended sets of organic tracers, in order to cover different types of urban conditions (Mediterranean, Continental, and Alpine), source types, and PM fractions. Our findings reveal that the vehicle exhaust source resulted to be less sensitive to the choice of analytes, although source contributions estimates can deviate significantly up to 44 %. On the other hand, for the detection of the non-exhaust one is clearly necessary to analyze specific inorganic elements. The choice of not analysing non-polar organics likely causes the loss of separation of exhaust and non-exhaust factors, thus obtaining a unique road traffic source, which provokes a significant bias of total contribution. Levoglucosan was, in most cases, crucial to identify biomass burning contributions in Milan and in Barcelona, in spite of the presence of PAHs in Barcelona, while for the case of Grenoble, even discarding levoglucosan, the presence of PAHs allowed identifying the BB factor. Modifying the rest of analytes provoke a systematic underestimation of biomass burning source contributions. SIA factors resulted to be generally overestimated with respect to the base case analysis, also in the case that ions were not included in the PMF analysis. Trace elements were crucial to identify shipping emissions (V and Ni) and industrial sources (Pb, Ni, Br, Zn, Mn, Cd and As). When changing the rest of input variables, the uncertainty was narrow for shipping but large for industrial processes. Major and trace elements were also crucial to identify the mineral/soil factor at all cities. Biogenic SOA and Anthropogenic SOA factors were sensitive to the presence of their molecular tracers, since the availability of OC alone is unable to separate a SOA factor. Arabitol and sorbitol were crucial to detecting fungal spores while odd number of higher alkanes (C27 to C31) for plant debris.

Temporal evolution and source apportionment of BC aerosols during autumn in the grassland of Ordos, China

AbstractMeteorological conditions and source emissions in grassland areas are quite different from those in urban areas, which significantly impacts the spatiotemporal characteristics of black carbon (BC). To obtain the characteristics of BC in the typical grassland environment in China, continuous observations of BC were carried out in Etuoke Banner, a typical grassland environment in Ordos, from September 8 to December 1, 2022. BC in Etuoke Banner in autumn is 22.4–4667.5 ng m−3, and the average concentration is 456.6 ng m−3, accounting for 2.20% of the mass fraction of PM2.5. BCliquid (BC generated from the combustion of liquid fuels) is the main component of BC (accounting for 79.2%); the average concentration is 361.7 ng m−3. The diurnal variations of BC, BCliquid, and BCsolid (BC generated from the combustion of solid fuels) are bimodal, with peaks at 08:00 and 18:00. The first peak is mainly related to traffic sources, cooking sources, and incomplete combustion of carbon‐containing substances; the second peak may be caused by emissions from residential cooking sources under the influence of meteorological conditions unfavorable to diffusion. The diurnal variation of absorption Ångström exponent (AAE) is unimodal, with the peak at 14:00. With the increase in BC mass concentration, AAE and visibility gradually decreased, wind speed first decreased and then increased, P and RH gradually increased, and the contribution of biomass combustion sources to BC decreased. In contrast, the contribution of traffic sources to BC increased. The evolution characteristics of atmospheric pollutants differed with the increase in BC concentration. The potential sources and affecting areas of BC and PM2.5 are mainly concentrated around Etuoke Banner and can affect the North China Plain after 48 h of transmission.

Development of a source-specific biomass burning emissions inventory for Washington, Oregon, and California

While wildfires are the dominant source of biomass burning emissions across the U.S., prescribed and agricultural burns also contribute to emissions and ambient air quality. Understanding the differential impacts that these different sources of biomass burning have on air quality and public health is important in the development of effective exposure reduction strategies. We leverage the high-resolution Fire INventory from NCAR (FINN) to develop a source-specific biomass burning emission inventory that distinguishes between wildfire, prescribed burn, and agricultural burn sources across Washington, Oregon, and California. We describe the methodology for reclassifying FINN using multiple national and state-level fire and fuel treatment inventories and present the results of the emissions reclassification process for these three states from 2012 to 2020. We matched 72%, 78% and 81% of FINN emissions event locations to fire locations from the fire type input datasets in Washington, Oregon, and California, respectively. When compared to county-level fire type-specific PM2.5 emissions estimates from the 2014, 2017, and 2020 EPA National Emissions Inventory, we found greater agreement among wildfire-specific estimates across years and states (R2 range: 0.59–0.98), relative to prescribed (R2 range: 0.12–0.73) and agricultural burns (R2 range: 0.43–0.95). This fire type-specific biomass burning emissions inventory can be used in air pollution transport models to better understand the impacts of each of these sources on air quality across the region along with downstream public health impacts.

Using PMF model and Bayesian model to quantify NOx sources in non-typhoons and Super Typhoon Lekima (2019) in Hangzhou

Quantifying and comparing nitrate (NO3−) sources in typhoons and non-typhoons is important for controlling and reducing their emissions. In this study, the chemical compositions and stable isotopes (δ15N–NO3- and δ18O–NO3-) of non-typhoon and Typhoon Lekima precipitation in Hangzhou (from May–August during 2019 and 2020) were determined. The results revealed that severe acid rain occurred in Hangzhou, except during Typhoon Lekima. According to the positive matrix factorization (PMF) model results, the ion contributions of sources in non-typhoons were as follows: secondary inorganic aerosols + biomass burning > sea salt aerosols > agricultural sources > terrestrial sources, whereas sea salt aerosols + biomass burning were the primary contributors of ions in Typhoon Lekima. The δ15N–NO3- values of non-typhoon and Typhoon Lekima ranged from −4.0 to −1.3‰ and −2.7 to 5.8‰, respectively. The δ18O–NO3- values of non-typhoon and Typhoon Lekima ranged from 56.3‰ to 74.7‰ and 32.2–55.3‰, respectively. The calculated contribution of N2O5 pathway in NOx oxidation to NO3− during non-typhoon precipitation was 64.7 ± 12.2%. If the contribution of OH· pathway during Typhoon Lekima precipitation was 87%, the Monte Carlo simulation results demonstrated that the estimated oxidation proportions of NO via O3 and RO2 (or HO2) ranged from 48.8 to 100% and 0–51.2%, respectively. Based on the improved Bayesian model combined with nitrogen isotope fractionation, the NOx contributions from four sources (biomass burning > coal combustion > mobile sources > microbial N cycle) in non-typhoon precipitation ranged from 21 to 30% (Ԑ = 3.6). In Typhoon Lekima (Ԑ = 5.2), lightning (23.6 ± 11.2%) was one of the primary NOx contributors and a lower contribution from microbial N cycle (17.9 ± 5.4%) compared with the PMF model (22.8%). Moreover, for Typhoon Lekima, the sum of biomass burning, coal combustion, and mobile sources in the improved Bayesian model (58.5%) was slightly lower than that of secondary inorganic aerosols in the PMF model (62.4%). Therefore, the coupled PMF–improved Bayesian model is a feasible and reliable method for source identification and apportionment of NO3− in precipitation.