scholarly journals Characterization of primary and aged wood burning and coal combustion organic aerosols in an environmental chamber and its implications for atmospheric aerosols

2021 ◽  
Vol 21 (13) ◽  
pp. 10273-10293
Author(s):  
Amir Yazdani ◽  
Nikunj Dudani ◽  
Satoshi Takahama ◽  
Amelie Bertrand ◽  
André S. H. Prévôt ◽  
...  
Keyword(s):  
Atmospheric Aerosols ◽  
Coal Combustion ◽  
Functional Group ◽  
Organic Aerosol ◽  
High Abundance ◽  
High Time Resolution ◽  
Environmental Chamber ◽  
Mir Spectroscopy ◽  
Wood Burning ◽  
Mir Spectra

Abstract. Particulate matter (PM) affects visibility, climate, and public health. Organic matter (OM), a uniquely complex portion of PM, can make up more than half of total atmospheric fine PM mass. We investigated the effect of aging on secondary organic aerosol (SOA) concentration and composition for wood burning (WB) and coal combustion (CC) emissions, two major atmospheric OM sources, using mid-infrared (MIR) spectroscopy and aerosol mass spectrometry (AMS). For this purpose, primary emissions were injected into an environmental chamber and aged using hydroxyl (diurnal aging) and nitrate (nocturnal aging) radicals to reach an atmospherically relevant oxidative age. A time-of-flight AMS instrument was used to measure the high-time-resolution composition of non-refractory fine PM, while fine PM was collected on PTFE filters before and after aging for MIR analysis. AMS and MIR spectroscopy indicate an approximately 3-fold enhancement of organic aerosol (OA) concentration after aging (not wall-loss corrected). The OM:OC ratios also agree closely between the two methods and increase, on average, from 1.6 before aging to 2 during the course of aging. MIR spectroscopy, which is able to differentiate among oxygenated groups, shows a distinct functional group composition for aged WB (high abundance of carboxylic acids) and CC OA (high abundance of non-acid carbonyls) and detects aromatics and polycyclic aromatic hydrocarbons (PAHs) in emissions of both sources. The MIR spectra of fresh WB and CC aerosols are reminiscent of their parent compounds with differences in specific oxygenated functional groups after aging, consistent with expected oxidation pathways for volatile organic compounds (VOCs) of each emission source. The AMS mass spectra also show variations due to source and aging that are consistent with the MIR functional group (FG) analysis. Finally, a comparison of the MIR spectra of aged chamber WB OA with that of ambient samples affected by residential wood burning and wildfires reveals similarities regarding the high abundance of organics, especially acids, and the visible signatures of lignin and levoglucosan. This finding is beneficial for the source identification of atmospheric aerosols and interpretation of their complex MIR spectra.

scholarly journals Characterization of primary and aged wood burning and coal combustion organic aerosols in environmental chamber and its implications for atmospheric aerosols

2020 ◽  
Author(s):  
Amir Yazdani ◽  
Nikunj Dudani ◽  
Satoshi Takahama ◽  
Amelie Bertrand ◽  
André S. H. Prévôt ◽  
...  
Keyword(s):  
Atmospheric Aerosols ◽  
Coal Combustion ◽  
Functional Group ◽  
Organic Aerosol ◽  
High Abundance ◽  
High Time Resolution ◽  
Environmental Chamber ◽  
Mir Spectroscopy ◽  
Wood Burning ◽  
Mir Spectra

Abstract. Particulate matter (PM) affects visibility, climate, and public health. Organic matter (OM), a uniquely complex portion of PM, can make up more than half of total atmospheric fine PM. We investigated the effect of aging on secondary organic aerosol (SOA) concentration and composition for wood burning (WB) and coal combustion (CC) emissions, two major atmospheric OM sources, using mid-infrared (MIR) spectroscopy and aerosol mass spectrometry (AMS). For this purpose, primary aerosols were injected into an environmental chamber and aged using hydroxyl (diurnal aging) and nitrate (nocturnal aging) radicals to reach an atmospherically-relevant oxidative age. A time-of-flight AMS instrument was used to measure high-time-resolution composition of non-refractory fine PM, while fine PM was collected on PTFE filters before and after aging for MIR analysis. AMS and MIR spectroscopy indicate an approximately three-fold enhancement of organic aerosol (OA) concentration after aging (not wall-loss corrected). The OM : OC ratios also agree closely between the two methods and increase, on average, from 1.6, before aging, to 2, during the course of aging. MIR spectroscopy, which is able to differentiate among oxygenated groups, shows a distinct functional group composition for aged WB (high abundance of carboxylic acids) and CC OA (high abundance of non-acid carbonyls) and detects aromatics and polycyclic aromatic hydrocarbons (PAHs) in emissions of both sources. The MIR spectra of fresh WB and CC aerosols are reminiscent of their parent compounds with differences in specific oxygenated functional groups after aging, consistent with expected oxidation pathways for volatile organic compounds (VOCs) of each emission source. The AMS mass spectra also show variations with source and aging that are consistent the MIR functional group (FG) analysis. Finally, comparison of the MIR spectra of chamber WB OA with that of ambient samples affected by residential wood burning and wildfires reveals similarities regarding the high abundance of organics, especially acids, and visible signatures of lignin and levoglucosan. This finding is beneficial to source identification of atmospheric aerosols and interpretation of their complex MIR spectra.

Organic functional group composition of particulate matter from fresh and aged wood burning and coal combustion

2020 ◽  
Author(s):  
Amir Yazdani ◽  
Nikunj Dudani ◽  
Satoshi Takahama ◽  
Amelie Bertrand ◽  
André S. H. Prévôt ◽  
...  
Keyword(s):  
Infrared Spectroscopy ◽  
Particulate Matter ◽  
Infrared Spectra ◽  
Atmospheric Aerosols ◽  
Coal Combustion ◽  
Organic Aerosol ◽  
High Abundance ◽  
Mid Infrared ◽  
Aerosol Mass ◽  
Wood Burning

<p>Particulate matter (PM) affects visibility and climate through light scattering, direct and indirect radiative forcing, and affecting cloud formation [1]. In addition, exposure to ambient fine PM is estimated to have caused 8.9 million deaths worldwide in 2015 [2]. Organic matter (OM), can make up more than half of total fine atmospheric PM, and yet its composition, formation mechanisms, and adverse health effects are not fully characterized due to its sheer compositional complexity. Biomass burning (e.g., residential wood burning, wildfires, and prescribed burning) and coal combustion (for heat and power generation) are two major OM sources, for which the impact of atmospheric aging - including secondary organic aerosol (SOA) formation - is not yet fully clear [3].</p><p>In this study, we investigated the effect of aging on composition and mass concentration of organic aerosols of wood burning (WB) and coal combustion (CC) emissions using two complementary methods, i.e., mid-infrared spectroscopy and aerosol mass spectrometry (AMS). For this purpose, primary aerosols were injected into the Paul Scherrer Institute (PSI) environmental chamber and aged using hydroxyl and nitrate radicals to simulate day-time and night-time oxidation processes in the atmosphere. In these experiments, aerosols reached an oxidative age comparable to that of atmospheric aerosols. A time-of-flight AMS instrument was used to measure the high-time-resolution composition of non-refractory fine PM, while we collected PM<sub>1 </sub>aerosols on PTFE filters before and after four hours of aging for off-line Fourier transform-infrared spectroscopy (FT-IR) measurements.</p><p>AMS and FT-IR estimates of organic aerosol mass concentration were highly correlated (r<sup>2</sup>=0.92); both indicating an approximately three-fold increase in organic aerosol concentration after aging. The OM/OC ratio, indicating the extent of oxidation also agreed closely between the two instruments and increased, on average, from 1.6 (before aging) to 2 (after aging). Mid-infrared spectroscopy, which is able to differentiate among oxygenated species, shows a distinct functional group composition for aged WB aerosols (high abundance of carboxylic acids) and CC aerosols (high abundance of non-acid carbonyls) and detects considerable amounts polycyclic aromatic hydrocarbons (PAHs) for both sources. Mid-infrared spectra of fresh WB and CC aerosols are reminiscent of their parent compounds with differences in specific functional groups suggesting the dominant oxidation pathways for each emission source. Finally, the comparison of mid-infrared spectra of aged WB aerosols in the environmental chamber with that of ambient samples affected by residential wood burning and wildfires reveals interesting similarities regarding the high abundance of alcohols and visible signatures of lignin. This finding is useful for interpreting sources of atmospheric aerosols and better interpretation of their complex mid-infrared spectra.</p><p>--------------------------</p><p>REFERENCES</p><p>[1] M. Hallquist et al., “The formation, properties and impact of secondary organic aerosol: current and emerging issues,” Atmos Chem Phys, 2009.</p><p>[2] R. Burnett et al., “Global estimates of mortality associated with long-term exposure to outdoor fine particulate matter,” Proc. Natl. Acad. Sci., 2018.</p><p>[3] A. Bertrand et al., “Primary emissions and secondary aerosol production potential from woodstoves for residential heating: Influence of the stove technology and combustion efficiency,” Atmos. Environ., 2017.</p>

scholarly journals Characterization of primary and secondary wood combustion products generated under different burner loads

2015 ◽  
Vol 15 (5) ◽  
pp. 2825-2841 ◽  
Author(s):  
E. A. Bruns ◽  
M. Krapf ◽  
J. Orasche ◽  
Y. Huang ◽  
R. Zimmermann ◽  
...  
Keyword(s):  
Gas Phase ◽  
Atmospheric Aerosols ◽  
Organic Aerosol ◽  
Combustion Products ◽  
High Load ◽  
Oxidation Products ◽  
Wood Combustion ◽  
Average Load ◽  
Wood Burning ◽  
Secondary Wood

Abstract. Residential wood burning contributes to the total atmospheric aerosol burden; however, large uncertainties remain in the magnitude and characteristics of wood burning products. Primary emissions are influenced by a variety of parameters, including appliance type, burner wood load and wood type. In addition to directly emitted particles, previous laboratory studies have shown that oxidation of gas-phase emissions produces compounds with sufficiently low volatility to readily partition to the particles, forming considerable quantities of secondary organic aerosol (SOA). However, relatively little is known about wood burning SOA, and the effects of burn parameters on SOA formation and composition are yet to be determined. There is clearly a need for further study of primary and secondary wood combustion aerosols to advance our knowledge of atmospheric aerosols and their impacts on health, air quality and climate. For the first time, smog chamber experiments were conducted to investigate the effects of wood loading on both primary and secondary wood combustion products. Products were characterized using a range of particle- and gas-phase instrumentation, including an aerosol mass spectrometer (AMS). A novel approach for polycyclic aromatic hydrocarbon (PAH) quantification from AMS data was developed and results were compared to those from GC-MS analysis of filter samples. Similar total particle mass emission factors were observed under high and average wood loadings; however, high fuel loadings were found to generate significantly higher contributions of PAHs to the total organic aerosol (OA) mass compared to average loadings. PAHs contributed 15 ± 4% (mean ±2 sample standard deviations) to the total OA mass in high-load experiments, compared to 4 ± 1% in average-load experiments. With aging, total OA concentrations increased by a factor of 3 ± 1 for high load experiments compared to 1.6 ± 0.4 for average-load experiments. In the AMS, an increase in PAH and aromatic signature ions at lower m / z values, likely fragments from larger functionalized PAHs, was observed with aging. Filter samples also showed an increase in functionalized PAHs in the particles with aging, particularly oxidized naphthalene species. As PAHs and their oxidation products are known to have deleterious effects on health, this is a noteworthy finding to aid in the mitigation of negative wood burning impacts by improving burner operation protocols.

scholarly journals Aging of atmospheric aerosols and the role of iron in catalyzing brown carbon formation

2021 ◽  
Author(s):  
Hind A. A. Al-Abadleh
Keyword(s):  
Volatile Organic Compounds ◽  
Organic Compounds ◽  
Atmospheric Aerosols ◽  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Atmospheric Oxidation ◽  
Carbon Formation ◽  
Brown Carbon ◽  
Volatile Organic

Extensive research has been done on the processes that lead to the formation of secondary organic aerosol (SOA) including atmospheric oxidation of volatile organic compounds (VOCs) from biogenic and anthropogenic...

scholarly journals Mid-Infrared Spectroscopy as a Rapid Tool to Qualitatively Predict the Effects of Species, Regions and Roasting on the Nutritional Composition of Australian Acacia Seed Species

Molecules ◽  
2021 ◽  
Vol 26 (7) ◽  
pp. 1879
Author(s):  
Oladipupo Q. Adiamo ◽  
Yasmina Sultanbawa ◽  
Daniel Cozzolino
Keyword(s):  
Principal Component ◽  
Nutritional Composition ◽  
Human Consumption ◽  
Mid Infrared ◽  
Mir Spectroscopy ◽  
As Species ◽  
Before And After ◽  
Mir Spectra ◽  
Main Components ◽  
Rapid Tool

In recent times, the popularity of adding value to under-utilized legumes have increased to enhance their use for human consumption. Acacia seed (AS) is an underutilized legume with over 40 edible species found in Australia. The study aimed to qualitatively characterize the chemical composition of 14 common edible AS species from 27 regions in Australia using mid-infrared (MIR) spectroscopy as a rapid tool. Raw and roasted (180 °C, 5, 7, and 9 min) AS flour were analysed using MIR spectroscopy. The wavenumbers (1045 cm−1, 1641 cm−1, and 2852–2926 cm−1) in the MIR spectra show the main components in the AS samples. Principal component analysis (PCA) of the MIR data displayed the clustering of samples according to species and roasting treatment. However, regional differences within the same AS species have less of an effect on the components, as shown in the PCA plot. Statistical analysis of absorbance at specific wavenumbers showed that roasting significantly (p < 0.05) reduced the compositions of some of the AS species. The results provided a foundation for hypothesizing the compositional similarity and/or differences among AS species before and after roasting.

scholarly journals Mitigation of Secondary Organic Aerosol Formation from Log Wood Burning Emissions by Catalytic Removal of Aromatic Hydrocarbons

2018 ◽  
Vol 52 (22) ◽  
pp. 13381-13390 ◽  
Author(s):  
Simone M. Pieber ◽  
Anastasios Kambolis ◽  
Davide Ferri ◽  
Deepika Bhattu ◽  
Emily A. Bruns ◽  
...  
Keyword(s):  
Aromatic Hydrocarbons ◽  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Aerosol Formation ◽  
Wood Burning ◽  
Secondary Organic Aerosol Formation ◽  
Catalytic Removal

scholarly journals Technical Note: Relating functional group measurements to carbon types for improved model-measurement comparisons of organic aerosol composition

2016 ◽  
Author(s):  
Satoshi Takahama ◽  
Giulia Ruggeri
Keyword(s):  
Organic Carbon ◽  
Functional Group ◽  
Organic Aerosol ◽  
Chem Phys ◽  
Technical Note ◽  
Molecular Structures ◽  
Organic Carbon Content ◽  
Aerosol Composition ◽  
Ft Ir ◽  
Model Measurement

Abstract. Functional group (FG) analysis provides a means by which functionalization in organic aerosol can be attributed to the abundances of its underlying molecular structures. However, performing this attribution requires additional, unobserved details about the molecular mixture to provide constraints in the estimation process. To address this issue, we present an approach for conceptualizing FG measurements of organic aerosol in terms of its functionalized carbon atoms. This reformulation facilitates estimation of mass recovery and biases in popular carbon-centric metrics that describe the extent of functionalization (such as oxygen to carbon ratio, organic mass to organic carbon mass ratio, and mean carbon oxidation state) for any given set of molecules and FGs analyzed. Furthermore, this approach allows development of parameterizations to more precisely estimate the organic carbon content from measured FG abundance. We use simulated photooxidation products of α-pinene secondary organic aerosol previously reported by Ruggeri et al. (Atmos. Chem. Phys., 16, 4401–4422, 2016) and FG measurements by Fourier Transform Infrared (FT-IR) spectroscopy in chamber experiments by Sax et al. (Aerosol Sci. Tech., 39, 822–830, 2005) to infer the relationships among molecular composition, FG composition, and metrics of organic aerosol functionalization. We find that for this simulated system, ~ 80 % of the carbon atoms should be detected by FGs for which calibration models are commonly developed, and ~ 7 % of the carbon atoms are undetectable by FT-IR analysis because they are not associated with vibrational modes in the infrared. Estimated biases due to undetected carbon fraction for these simulations are used to make adjustments in these carbon-centric metrics such that model-measurement differences are framed in terms of unmeasured heteroatoms (e.g., in hydroperoxide and nitrate groups for the case studied in this demonstration). The formality of this method provides framework for extending FG analysis to not only model-measurement but also instrument intercomparisons in other chemical systems.

scholarly journals Constraining condensed-phase formation kinetics of secondary organic aerosol components from isoprene epoxydiols

2016 ◽  
Vol 16 (3) ◽  
pp. 1245-1254 ◽  
Author(s):  
T. P. Riedel ◽  
Y.-H. Lin ◽  
Z. Zhang ◽  
K. Chu ◽  
J. A. Thornton ◽  
...  
Keyword(s):  
Aqueous Phase ◽  
Atmospheric Aerosols ◽  
Rate Constants ◽  
Reaction Rate ◽  
Secondary Organic Aerosol ◽  
Organic Aerosol ◽  
Heterogeneous Reactions ◽  
Model Calculations ◽  
Reaction Rate Constants ◽  
Aerosol Mass

Abstract. Isomeric epoxydiols from isoprene photooxidation (IEPOX) have been shown to produce substantial amounts of secondary organic aerosol (SOA) mass and are therefore considered a major isoprene-derived SOA precursor. Heterogeneous reactions of IEPOX on atmospheric aerosols form various aerosol-phase components or "tracers" that contribute to the SOA mass burden. A limited number of the reaction rate constants for these acid-catalyzed aqueous-phase tracer formation reactions have been constrained through bulk laboratory measurements. We have designed a chemical box model with multiple experimental constraints to explicitly simulate gas- and aqueous-phase reactions during chamber experiments of SOA growth from IEPOX uptake onto acidic sulfate aerosol. The model is constrained by measurements of the IEPOX reactive uptake coefficient, IEPOX and aerosol chamber wall losses, chamber-measured aerosol mass and surface area concentrations, aerosol thermodynamic model calculations, and offline filter-based measurements of SOA tracers. By requiring the model output to match the SOA growth and offline filter measurements collected during the chamber experiments, we derive estimates of the tracer formation reaction rate constants that have not yet been measured or estimated for bulk solutions.

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