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

Yazdani, Amir; Dudani, Nikunj; Takahama, Satoshi; Bertrand, Amélie; Prévôt, A. S. H.; Haddad, Imad El; Dillner, Ann M.

doi:10.5194/amt-2021-186

Cited by 2 publications

(1 citation statement)

References 49 publications

(64 reference statements)

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“…This is because the increase in the concentration of some mass fragments owing to SOA condensation might outweigh the decay for the same fragments generated by bbPOA oxidation or evaporation. This can especially render the loss of small oxygenated fragments that are common to several species (Yazdani et al, 2021b) undetectable by the method. For instance in experiment 4, levoglucosan-marker fragments, C 2 H 4 O 2 + , and C 3 H 5 O 2 + , decrease the most with aging.…”

Section: Aging By Uvmentioning

confidence: 99%

Chemical evolution of primary and secondary biomass burning aerosols during daytime and nighttime

Yazdani

Takahama

Kodros

et al. 2022

Preprint

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Abstract. Primary emissions from wood and pellet stoves were aged in an atmospheric simulation chamber under daytime and nighttime conditions. The aerosol was analyzed with the online Aerosol Mass Spectrometer (AMS) and offline Fourier transform infrared spectroscopy (FTIR). Measurements using the two techniques agreed reasonably well in terms of the organic aerosol (OA) mass concentration, OA:OC trends, and concentrations of biomass burning markers – lignin-like compounds and anhydrosugars. Based on the AMS, around 15 % of the primary organic aerosol (POA) mass underwent some form of transformation during daytime oxidation conditions after 6–10 hours of atmospheric exposure. A lesser extent of transformation was observed during the nighttime oxidation. The decay of certain semi-volatile (e.g., levoglucosan) and less volatile (e.g., lignin-like) POA components was substantial during aging, highlighting the role of heterogeneous reactions and gas-particle partitioning. Lignin-like compounds were observed to degrade under both daytime and nighttime conditions, whereas anhydrosugars degraded only under daytime conditions. Among the marker mass fragments of primary biomass burning OA (bbPOA), heavy ones (higher m/z) were relatively more stable during aging. The biomass burning secondary OA (bbSOA) became more oxidized with continued aging and resembled those of aged atmospheric organic aerosols. The bbSOA formed during daytime oxidation was dominated by acids. Organonitrates were an important product of nighttime reactions in both humid and dry conditions. Our results underline the importance of changes to both the primary and secondary biomass burning aerosols during their atmospheric aging. Heavier AMS fragments seldomly used in atmospheric chemistry can be used as more stable tracers of bbPOA and in combination with the established levoglucosan marker, can provide an indication of the extent of bbPOA aging.

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Section: Aging By Uvmentioning

confidence: 99%

Chemical evolution of primary and secondary biomass burning aerosols during daytime and nighttime

Yazdani

Takahama

Kodros

et al. 2022

Preprint

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

et al. 2021

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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.

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

Cited by 2 publications

References 49 publications

Chemical evolution of primary and secondary biomass burning aerosols during daytime and nighttime

Chemical evolution of primary and secondary biomass burning aerosols during daytime and nighttime

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

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