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Probing the impact of a phytoplankton bloom on the chemistry of nascent sea spray aerosol using high-resolution mass spectrometry
Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för miljövetenskap. Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).ORCID-id: 0000-0001-6332-7658
Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för miljövetenskap. University of the Faroe Islands, Faroe Islands.ORCID-id: 0000-0002-6416-2522
Stockholm Univ, Dept Environm Sci, SE-10691 Stockholm, Sweden.
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Antal upphovsmän: 72022 (Engelska)Ingår i: Environmental Science: Atmospheres, E-ISSN 2634-3606, Vol. 2, nr 5, s. 1152-1169Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

Sea spray aerosol is the largest natural source of aerosol to Earth's atmosphere with significant impacts on climate. Despite this, estimates of the impact of sea spray aerosol on Earth's radiation budget are highly uncertain due to an overall lack of understanding of the physical and chemical factors controlling its composition. Critically, results from studies probing the importance of oceanic biological activity on the amount and type of organic matter present in nascent sea spray aerosol have been ambiguous. Some field studies have shown a relationship between the organic fraction of sea spray aerosol and oceanic primary productivity while others have reported no such relationships. Given this, we have probed the composition of seawater and nascent sea spray aerosol during a phytoplankton bloom in the North Atlantic using a novel liquid chromatography-mass spectrometry method. We observed that the composition of dissolved organic matter present in seawater changed as the phytoplankton bloom progressed over an 18 day period. Further, we observed changes to both the chemical composition of the organic matter present in seawater and the chemical composition of the organic matter present in the sea spray aerosol despite the organic matter mass fraction of the aerosol remaining unchanged. More specifically, we observed that the nascent sea spray aerosol became progressively more enriched in surface-active organic substances as the bloom progressed and that the sea spray aerosol had a distinct organic matter composition compared to the seawater. Thus, our work provides additional insight into the biological dependence of nascent sea spray aerosol composition.

Ort, förlag, år, upplaga, sidor
2022. Vol. 2, nr 5, s. 1152-1169
Nationell ämneskategori
Geovetenskap och relaterad miljövetenskap
Identifikatorer
URN: urn:nbn:se:su:diva-209446DOI: 10.1039/d2ea00028hISI: 000841140100001Scopus ID: 2-s2.0-85136522517OAI: oai:DiVA.org:su-209446DiVA, id: diva2:1696884
Tillgänglig från: 2022-09-19 Skapad: 2022-09-19 Senast uppdaterad: 2025-02-07Bibliografiskt granskad
Ingår i avhandling
1. Enrichment of biogenic and anthropogenic organic substances on sea spray aerosols
Öppna denna publikation i ny flik eller fönster >>Enrichment of biogenic and anthropogenic organic substances on sea spray aerosols
2022 (Engelska)Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)
Abstract [en]

The world’s oceans are the source of one of the most abundant types of natural aerosols, namely sea spray aerosols (SSA). By scattering solar radiation, SSA play a significant role in controlling the Earth’s radiation budget, while they are also involved in the formation of clouds, acting as cloud condensation nuclei (CCN). To understand the connection between biogeochemical processes occurring in the ocean and in the atmosphere, it is crucial to gain better insight into the detailed chemical composition of SSA, which broadly consists of sea salt and marine organic matter. The aim of this thesis is to (1) better understand the impact of ocean biological activity on the chemical composition of SSA and (2) improve the knowledge on the ability of SSA to transport different organic pollutants to the atmosphere. In Paper I it was shown that changes in the composition of marine organic matter during a phytoplankton bloom in the North Atlantic were clearly reflected in the composition of generated SSA. Increased chlorophyll a concentration in seawater was correlated with the presence of lipid-like compounds with high H/C and low O/C atomic ratios, and a consistent trend in chemical composition was observed for subsurface water, the surface microlayer, and generated SSA. Although the effect of biological processes on the composition of SSA organic matter was clear, in Paper II it was shown that during the phytoplankton bloom, the abundance of organic matter in SSA was fairly constant, without any significant influence on their CCN activity or the particle production flux. Paper III provided a mechanistic understanding of the enrichment of different cationic surfactants (CSs) in SSA through experiments conducted using a sea spray simulation chamber. It was shown that enrichment of the CSs was primarily driven by the alkyl chain length of the CSs but also affected by the different functional groups in the CSs. The highest enrichment of CSs on SSA was observed for quaternary amines followed by primary and tertiary amines. Interaction with dissolved humic acid was shown to decrease the enrichment of longer-chain amines while the enrichment was increased for shorter-chain ones. When the plunging jet flow rate was increased, enrichment in SSA was shown to increase, especially for lower water concentrations of surface-active compounds. The purpose of Paper IV was to improve the understanding of the enrichment behavior of perfluoroalkyl acids (PFAAs), which are strong anionic surfactants. Similar to CSs, it was shown that increasing the plunging jet flow increased the enrichment on SSA, from 43-88% for different PFAAs. The effect of different inorganic salts present in seawater on enrichment was also tested. Compared to chamber experiments prepared with ~35% NaCl water matrix, it was shown that the presence of other seawater ions, namely Ca2+ and Mg2+, increased the enrichment of some PFAAs, especially for those with longer perfluoroalkyl chains.

Ort, förlag, år, upplaga, sidor
Stockholm: Department of Materials and Environmental Chemistry, Stockholm University, 2022. s. 43
Nyckelord
Sea spray, Organic carbon, Dissolved organic matter, Phytoplankton bloom, Cationic surfactants, Perfluorinated alkyl acids, LC-MS, HRMS
Nationell ämneskategori
Analytisk kemi
Forskningsämne
analytisk kemi
Identifikatorer
urn:nbn:se:su:diva-210894 (URN)978-91-8014-096-6 (ISBN)978-91-8014-097-3 (ISBN)
Disputation
2022-12-16, Högbomsalen, Geovetenskapens hus, Svante Arrhenius väg 12, Stockholm, 10:00
Opponent
Handledare
Tillgänglig från: 2022-11-23 Skapad: 2022-11-01 Senast uppdaterad: 2022-11-24Bibliografiskt granskad

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Radoman, NikolaChristiansen, SigurdCousins, Ian T.Salter, Matthew E.

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Radoman, NikolaChristiansen, SigurdCousins, Ian T.Salter, Matthew E.
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Environmental Science: Atmospheres
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