Biomass Burning Particles Research Articles

Mixing state and evolutionary mechanism of oxalic acid homologs in Liaocheng, East China: Insights from seasonal and hourly observations

Oxalic acid (C2) is a significant tracer of secondary organic aerosols (SOA), yet its precursors, evolutionary processes, and formation mechanisms are not fully understood. This knowledge gap leads to uncertainties in evaluating the climate effect and global budget of SOA. Here we compared the size distribution, mixing fraction, and evolutionary mechanism of C2-containing particles between summer and winter. In summer, the number of C2 particles and their homologs decreased compared to winter. However, the proportion of C2 relative to the total number of determined particles increased, indicating that the summertime particles are more aged. Higher relative aerosol acidity (Rra) and lower in-situ pH (pHis) in summer suggest that particles are more acidic during this season. Correlation analysis and temporal variation characteristics suggest that from 9: 00 to 15: 00 in summer, C2 particles mostly originate from the photochemical decomposition of larger dicarboxylic aids, driven by O3 concentration. Conversely, from 16: 00 to 20: 00, C2 particles are predominantly formed through aqueous-phase oxidation, influenced by higher relative humidity (RH), aerosol liquid water content (ALWC), and acidity. Additionally, heavy metal particles were the predominant type of C2 particles, and C2 particles exhibited an opposite diurnal variation to Fe in summer, suggesting that the photolysis of iron oxalate complexes is an important sink of C2 particles during this period. In winter, biomass burning (BB) particles were the most abundant, and a robust correlation between levoglucosan and C2 particles indicated a substantial influence of BB on C2 particles. The aqueous generation of C2 particles from α-dicarbonyls driven by acidity was most effective when RH varied from 40% to 60% in the wintertime state of particles. These findings highlight the hourly and seasonal variations in the sources and evolutionary processes of SOA. Such variations must be considered in developing control measures and simulating the climate effect of SOA.

Extreme wildfires over northern Greece during summer 2023 – Part A: Effects on aerosol optical properties and solar UV radiation

In Mediterranean countries, such as Greece, the frequency of forest fires has increased in recent years, primarily due to the widespread impacts of climate change. At the end of August 2023, Greece experienced a record-breaking heatwave that triggered severe wildfire incidents, significantly impacting the atmospheric conditions of several cities, among them Thessaloniki. A significant number of wildfires occurred in northern Greece (Evros), burning thousands of hectares of the protected Dadia forest (Natura 2000) and releasing a significant load of smoke into the atmosphere. According to the European Strategy Forum on Research Infrastructures (ESFRI) a total area of 90,000ha was burnt collectively by the Evros extreme wildfires during August 2023. The emissions led to severely adverse air pollution conditions, causing reduced visibility across an extended eastern Mediterranean region for several days. In this work, we analyze the influence of the transported biomass burning particles on the aerosol properties in the free troposphere, as well as on the surface UV radiation levels over Thessaloniki during the last week of August 2023. The transported smoke plume was detected over the Laboratory of Atmospheric Physics (LAP) in Thessaloniki, approximately 240 km away from the burning area, from August 22nd to the 25th. During this period, the presence of smoke led to exceptionally increased levels of aerosol optical depth (AOD), reaching up to 3.4 at 340nm (the highest ever recorded in Thessaloniki), as well as high Ångström exponent (AE) values, peaking at 2.4 for the 440–870nm range, followed by high Fine Mode Fractions (FMFs), indicating the prevalence of fine-mode smoke aerosol particle. Moreover, during the event, the presence of the biomass burning aerosols led to a strong attenuation of the solar UV irradiance by up to 90 %, reaching unprecedented levels, similar of a solar eclipse. The primary goal of this study is to highlight the extensive impacts that wildfires have, which are anticipated to increase in frequency in the near future, due to the predicted rise in the rate of occurrence of summer heatwaves especially for Mediterranean areas and specifically for Greece. Furthermore, the great value of the synergistic monitoring of the event with ground-based remote sensing instrumentation, along with satellite aerosol observations and modeling tools, is made prominent.

Amino acids in the water-soluble and water-insoluble fractions of the aerosols at a forested site in Japan

In order to clarify the concentration levels and sources of the water-insoluble amino acids (WIAA) in aerosols that have been received little attention in previous studies and to discuss their potential impact on nitrogen deposition, the WIAA in the coarse-mode (d = 2.0–10 μm) and fine-mode (d < 2.0 μm) aerosols were measured at a forested site in Japan together with the water-soluble free and combined amino acids. The sum of the WIAA showed more than a 6-times higher concentration than that of the water-soluble amino acids in the coarse-mode range and a similar concentration to that in the fine-mode range, which suggests a significant contribution of the WIAA to the amino acids pool in aerosols. The WIAA were predominantly partitioned into the coarse-mode range. The concentration of the coarse-mode WIAA was the highest in the summer and a strong correlation was found between the coarse-mode WIAA and nss-K+ concentrations. These results suggest that plant debris and the associated materials are important sources for the coarse-mode WIAA and the increase in the suspension of these particulate materials caused the enhancement of the WIAA in the summer. Remarkably higher concentrations of the coarse-mode WIAA than the water-soluble amino acids would be caused by these particulate materials. In the fine-mode range, on the other hand, the concentration of the WIAA was the highest in the spring and strongly correlated with the fine-mode nss-K+ concentrations. The fine-mode WIAA would be mainly derived from the biomass burning particles. The coarse-mode WIAA were estimated to significantly contribute to the dry deposition flux of the total nitrogen. The present study implies a potential impact of the WIAA in the coarse aerosols on nitrogen deposition.

Mapping the constituent preference of tree species for capturing particulate matter on leaf surfaces using single-particle mass spectrometry and supervised machine learning

Respiratory health is negatively influenced by the dimensions and constituents of particulate matter (PM). Although mass concentration is widely acknowledged to be key to assessing dust retention by urban trees, the role of plant leaves in filtering PM from the urban atmosphere, particularly regarding the particle dimensions and chemical constituents of retained PM on the leaf, remains elusive. Here we combined single-particle aerosol mass spectrometry and a particle resuspension chamber to investigate how urban tree species capture PM constituents. Results indicate that leaves are efficient in capturing relatively larger particles (1.0–2.0 μm). Compositionally, airborne particles were mostly composed of elemental carbon (EC, 20%), organic carbon (OC, 17%), and secondary reaction products (13%). However, leaf surfaces revealed a preference for retaining crustal species, comprising 55% of captured particulates. Notably, specific tree species demonstrated varied affinities for different PM constituents: Osmanthus fragrans Lour. predominantly captured levoglucosan (LEV), indicative of its efficiency against biomass burning particles, whereas Cinnamomum camphora (L.) J.Presl and Sabina chinensis var. kaizuca W.C.Cheng & W.T.Wang were more effective in capturing heavy metals (HMs). XGBoost modelling identified indicator ions, e.g., CN−, NO3−, NO2−, PO3−, with SHAP values surpassing 0.035, suggesting a preferential adsorption of these ions among different tree species. These findings demonstrate that the particulate capture efficiency of urban tree species varies with species-specific leaf properties, particularly in their ability to selectively adsorb particles containing hazardous constituents such as LEV and HMs. This study provides a scientific basis for the strategic selection of tree species in urban forestry initiatives aimed at improving air quality and public health.

Spatiotemporal of Particulate Matter (PM2.5) and Ozone (O3) in Eastern Northeast Brazil

ABSTRACT This research examines particulate matter with a diameter of 2.5 micrometers (PM2.5) and ozone (O3) variation across the climatic mesoregions of Alagoas. Mean PM2.5 and O3 concentrations across three mesoregions were as follows: East (5.91; 44.22 μg.m−3), Hinterland (6.90; 44.18 μg.m−3), and Arid (7.03; 44.23 μg.m−3). Spatial and temporal variations were observed, with PM2.5 concentrations highest in the northwest (NW) and O3 concentrations in the east (E), influenced by local sources, weather, and transportation. Differences between rainy and dry years were noted, attributed to biomass burning and dust particle transport. This study establishes a baseline for understanding air quality, lacking monitoring stations, aiding policymaking. It provides insights into PM2.5 and O3 dynamics, with PM2.5 concentrations highest in the NW and lower O3 concentrations in the E. Temporal variations emphasize the need for dynamic monitoring. Positive correlations between PM2.5 and O3 highlight complex relationships. Practical implications include proactive policymaking and the necessity for monitoring stations. Rigorous statistical methodologies inform model selection, enhancing environmental data understanding. Despite changes in land use, studies on extreme probability distributions are limited, emphasizing the need for robust methodologies for environmental data analysis to address air pollution challenges effectively in Alagoas.

Characterization of biomass burning tracers in particulate matter at 12 sites in China: Significant increase of coal combustion emitted levoglucosan in northern China during winter

Biomass burning (BB) is the largest contributor to carbonaceous aerosols globally. Specific organic tracers can track BB particles and identify BB types. At present, there is limited information on the composition of BB tracers on a continental scale. In this study, we conducted year-round sampling of particulate matter (PM) at 12 sites in China. Nine BB tracers were measured in PM with aerodynamic diameters <1.1 μm (PM<1.1), in the range of 1.1–3.3 μm (PM1.1–3.3), and > 3.3 μm (PM>3.3). The annual average concentration of these nine BB tracers (∑9 BB tracers) in the total PM was 366 ng m−3 with the majority of levoglucosan (66 %). The concentration of ∑9 BB tracers was higher in northern China than in southern China, especially in winter. ∑9 BB tracers were most enriched in PM<1.1 (50–61 % in mass), followed by PM1.1–3.3 and PM>3.3. The highest concentrations of ∑9 BB tracers were observed in winter, while satellite-recorded fire spots were intensive in autumn and spring. The mismatch of seasonal trends between them indicated that the high levels of BB tracers in winter was not due to open BB. The composition of 4-hydroxybenzoic acid, syringic acid and vanillic acid suggested that the burning of crop residues and softwoods were the major BB types in China. The ratio of levoglucosan to mannosan could neither identify the major BB types in China nor distinguish between BB and coal combustion. Correlation analysis and the PMF model demonstrated that non-BB sources contributed 7 %–58 % to levoglucosan at the 12 sites, with coal combustion being the predominant non-BB source in China, especially in northern urban sites during winter. Our findings suggest that caution should be taken in application of these organic tracers to identify BB types and estimate BB aerosols.

Chemical and optical characterization of aqueous secondary organic aerosol generated by reaction of pyruvaldehyde with sodium sulfite

Organic sulfonates are major constituents and tracers for secondary organic aerosol (SOA). Based on sodium sulfite (Na2SO3) and pyruvaldehyde are main components in aqueous environments, their mixed solution is atomized to simulate atmospheric processes of formation aquous SOA (aqSOA) from liquid aerosol particles rich in Na2SO3 and pyruvaldehyde after water evaporation. Constituents and optics of aqSOA are characterized using mass and spectroscopic instruments in this study. Negative ion mass spectra of aqSOA detected by aerosol laser time-of-flight mass spectrometer appeare strong organic sulfonates' characteristic cleavage peaks of m/z = 32(S−), 48(SO−), 64 (SO2−) and 80(SO3−). UV–Vis spectra of extraction solution for aqSOA existe characteristic absorption peak of organic sulfonate' SO at 210 nm. Peaks of 1140 and 1034 cm−1 in infrared absorption spectra correspond to antisymmetric and symmetric stretching vibration peaks of SO3 group, while, peaks of 830 and 760 cm−1 refer to asymmetric and symmetric stretching vibration absorption peaks of C–S–O. Also, peaks at m/z = 125, 153, 169, 185, 235 and 243 are presented in electrospray ionization negative ion mass spectra of extraction solution. These indicate that 1-hydroxyethane sulfonate and other organic sulfonates are major products of aqueous reaction for Na2SO3 and pyruvaldehyde. Light absorption capacity of aqSOA is remarkably enhanced, mass absorption coefficient averaged in 200–600 nm (<MAC>) for aqSOA is reach to that of biomass burning particles, and gradually raises with increment concentration of Na2SO3. These results can offer experimental basis to study components and optics of organic sulfonates in aerosols under high humidity conditions in polluted areas.

Optical and Microphysical Properties of the Aerosols during a Rare Event of Biomass-Burning Mixed with Polluted Dust

A rare event of mixed biomass-burning and polluted dust aerosols was observed over Athens, Greece (37.9° N, 23.6° E), during 21–26 May 2014. This event was studied using a synergy of a 6-wavelength elastic-Raman-depolarization lidar measurements, a CIMEL sun photometer, and in situ instrumentation. The FLEXPART dispersion model was used to identify the aerosol sources and quantify the contribution of dust and black carbon particles to the mass concentration. The identified air masses were found to originate from Kazakhstan and Saharan deserts, under a rare atmospheric pressure system. The lidar ratio (LR) values retrieved from the Raman lidar ranged within 25–89 sr (355 nm) and 35–70 sr (532 nm). The particle linear depolarization ratio (δaer) ranged from 7 to 28% (532 nm), indicating mixing of dust with biomass-burning particles. The aerosol optical depth (AOD) values derived from the lidar ranged from 0.09–0.43 (355 nm) to 0.07–0.25 (532 nm). An inversion algorithm was used to derive the mean aerosol microphysical properties (mean effective radius (reff), single scattering albedo (SSA), and mean complex refractive index (m)) inside selected atmospheric layers. We found that reff was 0.12–0.51 (±0.04) µm, SSA was 0.94–0.98 (±0.19) (at 532 nm), while m ranged between 1.39 (±0.05) + 0.002 (±0.001)i and 1.63 (±0.05) + 0.008 (±0.004)i. The polarization lidar photometer networking (POLIPHON) algorithm was used to estimate the vertical profile of the mass concentration for the dust and non-dust components. A mean mass concentration of 15 ± 5 μg m−3 and 80 ± 29 μg m−3 for smoke and dust was estimated for selected days, respectively. Finally, the retrieved aerosol microphysical properties were compared with column-integrated sun photometer CIMEL data with good agreement.

Insights into the seasonal characteristics of single particle aerosols in Chengdu based on SPAMS

To investigate the seasonal characteristics in air pollution in Chengdu, a single particle aerosol mass spectrometry was used to continuously observe atmospheric fine particulate matter during one-month periods in summer and winter, respectively. The results showed that, apart from O3, the concentrations of other pollutants (CO, NO2, SO2, PM2.5 and PM10) were significantly higher in winter than in summer. All single particle aerosols were divided into seven categories: biomass burning (BB), coal combustion (CC), Dust, vehicle emission (VE), K mixed with nitrate (K-NO3), K mixed with sulfate and nitrate (K-SN), and K mixed with sulfate (K-SO4) particles. The highest contributions in both seasons were VE particles (24%). The higher contributions of K-SO4 (16%) and K-NO3 (10%) particles occurred in summer and winter, respectively, as a result of their different formation mechanisms. S-containing (K-SO4 and K-SN), VE, and BB particles caused the evolution of pollution in both seasons, and they can be considered as targets for future pollution reduction. The mixing of primary sources particles (VE, Dust, CC, and BB) with secondary components was stronger in winter than in summer. In summer, as pollution worsens, the mixing of primary sources particles with 62 [NO3]− weakened, but the mixing with 97 [HSO4]− increased. However, in winter, the mixing state of particles did not exhibit an obvious evolution rules. The potential source areas in summer were mainly distributed in the southern region of Sichuan, while in winter, besides the southern region, the contribution of the western region cannot be ignored.

Research on Pollutant Emission Characteristics of Typical Biomass-fired Boilers

The combustion of biomass fuel boilers not only produces inorganic pollutants such as carbon oxides, nitrogen oxides, sulfur compounds, but also organic pollutants such as VOCs and PAHs, which directly affect the global biogeochemical cycle and atmospheric changes. Compared with foreign countries, there is relatively less research and related standards on the emission of organic pollutants from biomass fuel boilers in China. Therefore, it is necessary to study the emission characteristics of organic pollutants from biomass boilers, which can provide reference for the establishment of organic pollutant emission standards for biomass fuel boilers in China.The emission characteristics of volatile organic compounds(VOCs) and polycyclic aromatic hydrocarbons(PAHs) organic pollutants in the flue gas of three typical biomass-fired boilers in Chongqing were studied, and the emission concentrations of particulate matter, sulfur dioxides(SO2), and nitrogen oxides(NOX) were measured.The results show that the sulfur dioxide emissions from the three types of biomass-fired boilersrs are lower than the local standards in Chongqing, while nitrogen oxides and particulate matter have a phenomenon of exceeding the emission limits of the local standards in Chongqing. The main components of VOCs emitted from biomass powder and biomass particle combustion are OVOCs and aromatic hydrocarbons, while the main components of VOCs emitted from wood biomass combustion are alkynes. The gas-solid distribution pattern of PAHs during the combustion of three types of biomass is basically consistent. Low ring PAHs are mainly enriched in the gas phase, while medium and high ring PAHs are mainly enriched in particulate matter.

Influence of Relative Humidity and Aging on Morphology and Chemical Composition on Biomass Burning Particle

Influence of Relative Humidity and Aging on Morphology and Chemical Composition on Biomass Burning Particle

Characterization of summertime single aerosol particles in Chengdu (China): Interannual evolution and impact of COVID-19 lockdown

To investigate the interannual evolution of air pollution in summer and the impact of the COVID-19 lockdown on local pollution in Chengdu, China, single aerosol particles were continuously measured in three summer periods: the regular period in 2020 (RP2020); the regular period in 2022 (RP2022); and the lockdown period in 2022 (LP2022). It was found that, from RP2020 to RP2022, the mass concentrations of PM2.5, PM10, SO2 and NO2 decreased by 25.6 %, 24.7 %, 28.8 % and 38.5 %, respectively, while the concentration of O3 increased by 11.0 %. Affected by regional transport, there was no significant decrease in the concentrations of various pollutants during LP2022. All single aerosol particles could be classified into seven categories: vehicle emissions (VE), dust, biomass burning (BB), coal combustion (CC), K mixed with sulfate (KSO4), K mixed with nitrate (KNO3) and K mixed with sulfate and nitrate (KSN) particles. From RP2020 to RP2022, the contributions of BB and CC particles decreased by 12.1 % and 0.9 %, respectively, while VE and dust particles increased by 3.6 % and 2.5 %, respectively; and compared to RP2022, the contributions of VE, dust and CC particles in LP2022 decreased by 22.2 %, 11.0 % and 12.7 %, respectively. The high PM2.5 pollution events in RP2020 and RP2022 were mainly caused by combustion sources (BB and CC, 51.6 %) and VE (38.3 %) particles, respectively, while the pollution event in LP2022 was contributed by BB (27.0 %) and secondary inorganic (KSO4, KNO3 and KSN, 60.2 %) particles. The formation mechanisms of different pollution events were further validated by WRF-Chem results. Although the potential source areas of particles showed a shrinking trend from RP2020 to RP2022, regional transport still caused high PM2.5 pollution events during LP2022. Photochemical processes dominated the formation of KSO4 particles, while the KNO3 and KSN particles were mainly generated by liquid-phase reactions, and this effect increased year by year.

The extreme forest fires in California/Oregon in 2020: Aerosol optical and physical properties and comparisons of aged versus fresh smoke

Wildfire activity in the western United States during August to October 2020 was exceptional in terms of the fire severity and area burned. Extremely dry biomass fuels from near historic multi-year drought conditions were further exacerbated with very hot and dry conditions in 2020. These conditions when coupled with strong offshore flow allowed many ignitions to grow into extremely large and severe wildfires. Long-term monitoring at a few AERONET sites in California showed that the number of days with high Aerosol Optical Depth at 440 nm (AOD440>1) in 2020 was greater than any other year going back to the beginning of the data records in 2002. A wide range of fine mode particle volume median radii were retrieved from AERONET data over the course of these fires suggesting significant variability in combustion conditions and aging processes. Additionally, the fine mode radii in some of these smoke plumes in 2020 were very large especially at high AOD (∼0.22–0.32 μm volume median radius), likely due to both coagulation and condensation occurring during aging at very high particulate concentrations. The largest fine mode particle radii combined with narrow distributions resulted in some very rare AOD spectra showing peak AOD at 500 nm and decreasing to lower AOD at both shorter and longer wavelengths. The most extreme retrieved size distributions and associated measured AOD spectra were principally observed in long-distance transported smoke plumes from these western United States fires at sites in Colorado, Maryland and Virginia, possibly due to further aging during transport. Additionally, strong absorption was sometimes observed at short wavelengths with much lower single scattering albedo at 440 nm compared to 675 nm in some plumes consistent with significant brown carbon (BrC) and/or coated black carbon (BC) absorption in biomass burning particles. This strong spectral absorption signature observed at some California sites and dates remained similarly strong in some smoke plumes observed at some east coast sites in Maryland and Virginia, thereby suggesting that the lifetime of these particular BrC and/or coated BC absorbing species was greater than 5 days.

Effect of turbulent mixing on combustion behaviours of a single biomass pellet

Biomass co-firing in coal-fired power plants is an appealing technology for reducing greenhouse gas emissions due to the abundant biomass resource and low cost of retrofitting the existing power plants. Burning larger biomass particles is inevitable in real boilers due to the energy-consuming grinding process. A profound understanding of the combustion characteristics of larger biomass particles in a strong turbulent gas environment inside the boiler is essential for designing and operating biomass conversion facilities. This paper presents a detailed experimental study of the effects of turbulent mixing on the combustion of biomass particles. An impinging arranged four-fan stirred turbulent furnace was established in the laboratory. Particle image velocimetry (PIV) was adopted to measure the turbulent flow field characteristics under various fan speeds. The combustion behaviours of a 5 mm homemade cylindrical cellulose pellet were investigated under natural convection and turbulent flow at 700 °C. The centre and surface temperature of the particle, the shape and peak temperature of the volatile flame, and the sequential combustion history were measured and analysed. The results show that the turbulent fluctuation velocity Velrms increases linearly with increasing fan speed. Whether the gas environment is natural convection or turbulence has an essential impact on the combustion behaviours of the biomass particle. Increasing turbulence intensity accelerates the heating rate and significantly shortens the burnout time from 94 s to 55 s. The volatile flame area fluctuates randomly and generally decreases with the turbulent intensity due to the dilution of gas-phase volatiles by the turbulent eddies motion. Volatile flame has higher local luminosity and peak combustion temperature at a low turbulent fluctuation velocity of 0 ∼ 0.8 m/s but gradually weakens due to heat dissipation at a higher turbulent fluctuation velocity of 0.8 ∼ 1.6 m/s. The present results are the first to study the combustion behaviours of a single biomass pellet in different turbulent intensities, indicating that the effect of enhanced heat and mass transfer in turbulent environments on biomass combustion is essential and deserves further study.

Dynamic Wood Smoke Aerosol Toxicity during Oxidative Atmospheric Aging.

Wildfires are a major source of biomass burning aerosol to the atmosphere, with their incidence and intensity expected to increase in a warmer future climate. However, the toxicity evolution of biomass burning organic aerosol (BBOA) during atmospheric aging remains poorly understood. In this study, we report a unique set of chemical and toxicological metrics of BBOA from pine wood smoldering during multiphase aging by gas-phase hydroxyl radicals (OH). Both the fresh and OH-aged BBOA show activity relevant to adverse health outcomes. The results from two acellular assays (DTT and DCFH) show significant oxidative potential (OP) and reactive oxygen species (ROS) formation in OH-aged BBOA. Also, radical concentrations in the aerosol assessed by electron paramagnetic resonance (EPR) spectroscopy increased by 50% following heterogeneous aging. This enhancement was accompanied by a transition from predominantly carbon-centered radicals (85%) in the fresh aerosol to predominantly oxygen-centered radicals (76%) following aging. Both the fresh and aged biomass burning aerosols trigger prominent antioxidant defense during the in vitro exposure, indicating the induction of oxidative stress by BBOA in the atmosphere. By connecting chemical composition and toxicity using an integrated approach, we show that short-term aging initiated by OH radicals can produce biomass burning particles with a higher particle-bound ROS generation capacity, which are therefore a more relevant exposure hazard for residents in large population centers close to wildfire regions than previously studied fresh biomass burning emissions.

Real-time, single-particle chemical composition, volatility and mixing state measurements of urban aerosol particles in southwest China

To investigate the volatility of atmospheric particulates and the evolution of other particulate properties (chemical composition, particle size distribution and mixing state) with temperature, a thermodenuder coupled with a single particle aerosol mass spectrometer was used to conduct continuous observations of atmospheric fine particles in Chengdu, southwest China. Because of their complex sources and secondary reaction processes, the average mass spectra of single particles contained a variety of chemical components (including organic, inorganic and metal species). When the temperature rose from room temperature to 280°C, the relative areas of volatile and semi-volatile components decreased, while the relative areas of less or non-volatile components increased. Most (> 80%) nitrate and sulfate existed in the form of NH4NO3 and (NH4)2SO4, and their volatilization temperatures were 50–100°C and 150–280°C, respectively. The contribution of biomass burning (BB) and vehicle emission (VE) particles increased significantly at 280°C, which emphasized the important role of regional biomass burning and local motor vehicle emissions to the core of particles. With the increase in temperature, the particle size of the particles coated with volatile or semi-volatile components was reduced, and their mixing with secondary inorganic components was significantly weakened. The formation of K-nitrate (KNO3) and K-sulfate (KSO4) particles was dominated by liquid-phase processes and photochemical reactions, respectively. Reducing KNO3 and BB particles is the key to improving visibility. These new results are helpful towards better understanding the initial sources, pollution formation mechanisms and climatic effects of fine particulate matter in this megacity in southwest China.

Ambient particle characteristics by single particle aerosol mass spectrometry at a coastal site in Hong Kong: a case study affected by the sea-land breeze.

The sea-land breeze (SLB) circulation plays a vital role in the transport of atmospheric pollutants in coastal cities. In this study, a single particle aerosol mass spectrometer (SPAMS) and combined bulk aerosol instruments were deployed to investigate the ambient particle characteristic at a suburban coastal site in Hong Kong from February 22 to March 10, 2013. Significant SLB circulations were captured from March 6-10, 2013, during the campaign. During the SLB periods, air quality worsened, with PM2.5 concentrations reaching a peak of 55.6 μg m-3 and an average value of 42.8 ± 4.5 μg m-3. A total of 235,894 particles were measured during the SLB stage. Eight major sources were identified by investigating the mixing states of the total particles, including the coal-burning related particles (48.1%), biomass burning particles (6.7%), vehicle emission-related particles (16.4%), sea salt (9.2%), ship emission particles (2.7%), dust/steeling industries (3.7%), waste incineration (6.3%), and road dust (3.9%). It was noteworthy that the PM2.5 concentrations and particle numbers increased sharply during the transition of land wind to the sea breeze. Meanwhile, the continental sourced pollutants recirculated back to land resulting in a cumulative increase in pollutants. Both individual and bulk measurements support the above results, with high contributions from coal burning, biomass burning, bulk K+, and NO3 -, which were probably from the regional transportation from the nearby area. In contrast, the ship and vehicle emissions increased during the SLB period, with a high sulfate concentration partially originating from the ship emission. In this study, field evidence of continental-source pollutants backflow to land with the evolution of sea breeze was observed and helped our current understanding of the effect of SLB on air quality in the coastal city.

Associations between long-term exposures to airborne PM2.5 components and mortality in Massachusetts: mixture analysis exploration

Background:Numerous studies have documented PM2.5’s links with adverse health outcomes. Comparatively fewer studies have evaluated specific PM2.5 components. The lack of exposure measurements and high correlation among different PM2.5 components are two limitations.Methods:We applied a novel exposure prediction model to obtain annual Census tract-level concentrations of 15 PM2.5 components (Zn, V, Si, Pb, Ni, K, Fe, Cu, Ca, Br, SO42−, NO3−, NH4+, OC, EC) in Massachusetts from 2000 to 2015, to which we matched geocoded deaths. All non-accidental mortality, cardiovascular mortality, and respiratory mortality were examined for the population aged 18 or over. Weighted quantile sum (WQS) regression models were used to examine the cumulative associations between PM2.5 components mixture and outcomes and each component’s contributions to the cumulative associations. We have fit WQS models on 15 PM2.5 components and a priori identified source groups (heavy fuel oil combustion, biomass burning, crustal matter, non-tailpipe traffic source, tailpipe traffic source, secondary particles from power plants, secondary particles from agriculture, unclear source) for the 15 PM2.5 components. Total PM2.5 mass analysis and single component associations were also conducted through quasi-Poisson regression models.Results:Positive cumulative associations between the components mixture and all three outcomes were observed from the WQS models. Components with large contribution to the cumulative associations included K, OC, and Fe. Biomass burning, traffic emissions, and secondary particles from power plants were identified as important source contributing to the cumulative associations. Mortality rate ratios for cardiovascular mortality were of greater magnitude than all non-accidental mortality and respiratory mortality, which is also observed in cumulative associations estimated from WQS, total PM2.5 mass analysis, and single component associations.Conclusion:We have found positive associations between the mixture of 15 PM2.5 components and all non-accidental mortality, cardiovascular mortality, and respiratory mortality. Among these components, Fe, K, and OC have been identified as having important contribution to the cumulative associations. The WQS results also suggests potential source effects from biomass burning, traffic emissions, and secondary particles from power plants.

Canadian and Alaskan wildfire smoke particle properties, their evolution, and controlling factors, from satellite observations

Abstract. The optical and chemical properties of biomass burning (BB) smoke particles greatly affect the impact that wildfires have on climate and air quality. Previous work has demonstrated some links between smoke properties and factors such as fuel type and meteorology. However, the factors controlling BB particle speciation at emission are not adequately understood nor are the factors driving particle aging during atmospheric transport. As such, modeling wildfire smoke impacts on climate and air quality remains challenging. The potential to provide robust, statistical characterizations of BB particles based on ecosystem type and ambient environmental conditions with remote sensing data is investigated here. Space-based Multi-angle Imaging SpectroRadiometer (MISR) observations, combined with the MISR Research Aerosol (RA) algorithm and the MISR Interactive Explorer (MINX) tool, are used to retrieve smoke plume aerosol optical depth (AOD) and to provide constraints on plume vertical extent; smoke age; and particle size, shape, light-absorption properties, and absorption spectral dependence. These tools are applied to numerous wildfire plumes in Canada and Alaska, across a range of conditions, to create a regional inventory of BB particle-type temporal and spatial distribution. We then statistically compare these results with satellite measurements of fire radiative power (FRP) and land cover characteristics, as well as short-term climate, meteorological, and drought information from the Modern-Era Retrospective analysis for Research and Applications (MERRA-2) reanalysis and the North American Drought Monitor. We find statistically significant differences in the retrieved smoke properties based on land cover type, with fires in forests producing the thickest plumes containing the largest, brightest particles and fires in savannas and grasslands exhibiting the opposite. Additionally, the inferred dominant aging mechanisms and the timescales over which they occur vary systematically between land types. This work demonstrates the potential of remote sensing to constrain BB particle properties and the mechanisms governing their evolution over entire ecosystems. It also begins to realize this potential, as a means of improving regional and global climate and air quality modeling in a rapidly changing world.

A quadcopter unmanned aerial system (UAS)-based methodology for measuring biomass burning emission factors

Abstract. Biomass burning (BB) emits large quantities of greenhouse gases (GHG) and aerosols that impact the climate and adversely affect human health. Although much research has focused on quantifying BB emissions on regional to global scales, field measurements of BB emission factors (EFs) are sparse, clustered and indicate high spatio-temporal variability. EFs are generally calculated from ground or aeroplane measurements with respective potential biases towards smouldering or flaming combustion products. Unmanned aerial systems (UAS) have the potential to measure BB EFs in fresh smoke, targeting different parts of the plume at relatively low cost. We propose a light-weight UAS-based method to measure EFs for carbon monoxide (CO), carbon dioxide (CO2), methane (CH4), and nitrous oxide (N2O) as well as PM2.5 (TSI Sidepak AM520) and equivalent black carbon (eBC, microAeth AE51) using a combination of a sampling system with Tedlar bags which can be analysed on the ground and with airborne aerosol sensors. In this study, we address the main challenges associated with this approach: (1) the degree to which a limited number of samples is representative for the integral smoke plume and (2) the performance of the lightweight aerosol sensors. While aerosol measurements can be made continuously in a UAS set-up thanks to the lightweight analysers, the representativeness of our Tedlar bag filling approach was tested during prescribed burning experiments in the Kruger National Park, South Africa. We compared fire-averaged EFs from UAS-sampled bags for savanna fires with integrated EFs from co-located mast measurements. Both measurements matched reasonably well with linear R2 ranging from 0.81 to 0.94. Both aerosol sensors are not factory calibrated for BB particles and therefore require additional calibration. In a series of smoke chamber experiments, we compared the lightweight sensors with high-fidelity equipment to empirically determine specific calibration factors (CF) for measuring BB particles. For the PM mass concentration from a TSI Sidepak AM520, we found an optimal CF of 0.27, using a scanning mobility particle sizer and gravimetric reference methods, although the CF varied for different vegetation fuel types. Measurements of eBC from the Aethlabs AE51 aethalometer agreed well with the multi-wavelength aethalometer (AE33) (linear R2 of 0.95 at λ=880 nm) and the wavelength corrected multi-angle absorption photometer (MAAP, R2 of 0.83 measuring at λ=637 nm). However, the high variability in observed BB mass absorption cross-section (MAC) values (5.2±5.1 m2 g−1) suggested re-calibration may be required for individual fires. Overall, our results indicate that the proposed UAS set-up can obtain representative BB EFs for individual savanna fires if proper correction factors are applied and operating limitations are well understood.