Measurements of Atmospheric Proteinaceous Aerosol in the Arctic Using a Selective UHPLC/ESI-MS/MS Strategy

Rad, Farshid Mashayekhy; Zurita, Javier; Gilles, Philippe; Rutgeerts, Laurens A. J.; Nilsson, Ulrika; Ilag, Leopold L.; Leck, Caroline

doi:10.1007/s13361-018-2009-8

Cited by 17 publications

(21 citation statements)

References 48 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Amino acids and fatty acids have previously been observed in the SML of open leads in the summer high Arctic 61,62 and in bulk ambient aerosols during spring–summer in the Canadian Arctic 60,63 and during spring–fall at Svalbard. 64,65 Notably, all SSA particles containing amino acids also contained saccharides, and most particles (75%, by number) containing one short-chain fatty acid also contained a saccharide signature. Only 33% of particles matching saccharides did not contain any other organic type.…”

Section: Resultsmentioning

confidence: 99%

Wintertime Arctic Sea Spray Aerosol Composition Controlled by Sea Ice Lead Microbiology

et al. 2019

View full text Add to dashboard Cite

The Arctic is experiencing the greatest warming on Earth, as most evident by rapid sea ice loss. Delayed sea ice freeze-up in the Alaskan Arctic is decreasing wintertime sea ice extent and changing marine biological activity. However, the impacts of newly open water on wintertime sea spray aerosol (SSA) production and atmospheric composition are unknown. Herein, we identify SSA, produced locally from open sea ice fractures (leads), as the dominant aerosol source in the coastal Alaskan Arctic during winter, highlighting the year-round nature of Arctic SSA emissions. Nearly all of the individual SSA featured thick organic coatings, consisting of marine saccharides, amino acids, fatty acids, and divalent cations, consistent with exopolymeric secretions produced as cryoprotectants by sea ice algae and bacteria. In contrast, local summertime SSA lacked these organic carbon coatings, or featured thin coatings, with only open water nearby. The individual SSA composition was not consistent with frost flowers or surface snow above sea ice, suggesting that neither hypothesized frost flower aerosolization nor blowing snow sublimation resulted in the observed SSA. These results further demonstrate the need for inclusion of lead-based SSA production in modeling of Arctic atmospheric composition. The identified connections between changing sea ice, microbiology, and SSA point to the significance of sea ice lead biogeochemistry in altering Arctic atmospheric composition, clouds, and climate feedbacks during winter.

show abstract

Section: Resultsmentioning

confidence: 99%

Wintertime Arctic Sea Spray Aerosol Composition Controlled by Sea Ice Lead Microbiology

et al. 2019

View full text Add to dashboard Cite

show abstract

“…Concerning abiotic transformation (photo-transformation and radical chemistry) in atmospheric waters, some studies determined kinetic rate constants (k) of AAs with radicals (e.g., OH) (Scholes et al, 1965;Motohashi and Saito, 1993;Prütz and Vogel, 1976), singlet oxygen ( 1 O 2 ) (Kraljić and Sharpatyi, 1978;Matheson and Lee, 1979;McGregor and Anastasio, 2001;Michaeli and Feitelson, 1994;Miskoski and García, 1993;McGregor and Anastasio, 2001), or ozone (O 3 ) (Ignatenko and Cherenkevich, 1985;Pryor et al, 1984). Based on such kinetic data, some studies have reported the time of life of amino acids in fog (McGregor and Anastasio, 2001) or in cloud water (Triesch et al, 2021).…”

Section: Introductionmentioning

confidence: 99%

Biotic and abiotic transformation of amino acids in cloud water: experimental studies and atmospheric implications

et al. 2021

View full text Add to dashboard Cite

Abstract. The interest in organic nitrogen and particularly in quantifying and studying the fate of amino acids (AAs) has been growing in the atmospheric-science community. However very little is known about biotic and abiotic transformation mechanisms of amino acids in clouds. In this work, we measured the biotransformation rates of 18 amino acids with four bacterial strains (Pseudomonas graminis PDD-13b-3, Rhodococcus enclensis PDD-23b-28, Sphingomonas sp. PDD-32b-11, and Pseudomonas syringae PDD-32b-74) isolated from cloud water and representative of this environment. At the same time, we also determined the abiotic (chemical, OH radical) transformation rates within the same solutions mimicking the composition of cloud water. We used a new approach by UPLC–HRMS (ultra-performance liquid chromatography–high-resolution mass spectrometry) to quantify free AAs directly in the artificial-cloud-water medium without concentration and derivatization. The experimentally derived transformation rates were used to compare their relative importance under atmospheric conditions with loss rates based on kinetic data of amino acid oxidation in the aqueous phase. This analysis shows that previous estimates overestimated the abiotic degradation rates and thus underestimated the lifetime of amino acids in the atmosphere, as they only considered loss processes but did not take into account the potential transformation of amino acids into each other.

show abstract

“…In general, previous studies have shown that amino acids in aerosol particles can have both natural and anthropogenic sources. Having been detected in volcanic emissions (Scalabrin et al, 2012) and during biomass burning events (Chan et al, 2005;Feltracco et al, 2019), amino acids can be produced by plants, pollens, fungi, bacterial spores and algae (Milne and Zika, 1993;Zhang and Anastasio, 2003;Matos et al, 2016). Nevertheless, they are useful indicators for aerosol particle age and origin (Barbaro et al, 2011;Matsumoto and Uematsu, 2005;Scalabrin et al, 2012).…”

Section: Introductionmentioning

confidence: 99%

“…Although the study and characterization of amino acids are of paramount importance for atmospheric scientists, the true role and the fate of amino acids in the atmosphere are still poorly understood (Matos et al, 2016). Despite several studies of FAAs also conducted in the marine environment, there is still a huge uncertainty as to the question of whether FAAs are of marine origin or not.…”

Section: Introductionmentioning

confidence: 99%

Concerted measurements of free amino acids at the Cabo Verde islands: high enrichments in submicron sea spray aerosol particles and cloud droplets

et al. 2021

View full text Add to dashboard Cite

Abstract. Measurements of free amino acids (FAAs) in the marine environment to elucidate their transfer from the ocean into the atmosphere, to marine aerosol particles and to clouds, were performed at the MarParCloud (marine biological production, organic aerosol particles and marine clouds: a process chain) campaign at the Cabo Verde islands in autumn 2017. According to physical and chemical specifications such as the behavior of air masses, particulate MSA concentrations and MSA∕sulfate ratios, as well as particulate mass concentrations of dust tracers, aerosol particles predominantly of marine origin with low to medium dust influences were observed. FAAs were investigated in different compartments: they were examined in two types of seawater underlying water (ULW) and in the sea surface microlayer (SML), as well as in ambient marine size-segregated aerosol particle samples at two heights (ground height based at the Cape Verde Atmospheric Observatory, CVAO, and at 744 m height on Mt. Verde) and in cloud water using concerted measurements. The ∑FAA concentration in the SML varied between 0.13 and 3.64 µmol L−1, whereas it was between 0.01 and 1.10 µmol L−1 in the ULW; also, a strong enrichment of ∑FAA (EFSML: 1.1–298.4, average of 57.2) was found in the SML. In the submicron (0.05–1.2 µm) aerosol particles at the CVAO, the composition of FAAs was more complex, and higher atmospheric concentrations of ∑FAA (up to 6.3 ng m−3) compared to the supermicron (1.2–10 µm) aerosol particles (maximum of 0.5 ng m−3) were observed. The total ∑FAA concentration (PM10) was between 1.8 and 6.8 ng m−3 and tended to increase during the campaign. Averaged ∑FAA concentrations in the aerosol particles on Mt. Verde were lower (submicron: 1.5 ng m−3; supermicron: 1.2 ng m−3) compared to the CVAO. A similar contribution percentage of ∑FAA to dissolved organic carbon (DOC) in the seawater (up to 7.6 %) and to water-soluble organic carbon (WSOC) in the submicron aerosol particles (up to 5.3 %) indicated a related transfer process of FAAs and DOC in the marine environment. Considering solely ocean–atmosphere transfer and neglecting atmospheric processing, high FAA enrichment factors were found in both aerosol particles in the submicron range (EFaer(∑FAA): 2×103–6×103) and medium enrichment factors in the supermicron range (EFaer(∑FAA): 1×101–3×101). In addition, indications for a biogenic FAA formation were observed. Furthermore, one striking finding was the high and varying FAA cloud water concentration (11.2–489.9 ng m−3), as well as enrichments (EFCW: 4×103 and 1×104 compared to the SML and ULW, respectively), which were reported here for the first time. The abundance of inorganic marine tracers (sodium, methanesulfonic acid) in cloud water suggests an influence of oceanic sources on marine clouds. Finally, the varying composition of the FAAs in the different matrices shows that their abundance and ocean–atmosphere transfer are influenced by additional biotic and abiotic formation and degradation processes. Simple physicochemical parameters (e.g., surface activity) are not sufficient to describe the concentration and enrichments of the FAAs in the marine environment. For a precise representation in organic matter (OM) transfer models, further studies are needed to unravel their drivers and understand their composition.

show abstract

Measurements of Atmospheric Proteinaceous Aerosol in the Arctic Using a Selective UHPLC/ESI-MS/MS Strategy

Cited by 17 publications

References 48 publications

Wintertime Arctic Sea Spray Aerosol Composition Controlled by Sea Ice Lead Microbiology

Wintertime Arctic Sea Spray Aerosol Composition Controlled by Sea Ice Lead Microbiology

Biotic and abiotic transformation of amino acids in cloud water: experimental studies and atmospheric implications

Concerted measurements of free amino acids at the Cabo Verde islands: high enrichments in submicron sea spray aerosol particles and cloud droplets

Contact Info

Product

Resources

About