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Character and environmental lability of cyanobacteria-derived dissolved organic matter
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - BMC, Analytical Chemistry.ORCID iD: 0000-0002-4301-3923
Uppsala University, Disciplinary Domain of Science and Technology, Biology, Department of Cell and Molecular Biology, Molecular Evolution. Uppsala University, Science for Life Laboratory, SciLifeLab.ORCID iD: 0000-0002-2942-5390
Uppsala University, Disciplinary Domain of Science and Technology, Biology, Department of Ecology and Genetics, Limnology. Department of Ecology, Environment, and Plant Sciences, Science for Life Laboratory, Stockholm University, Stockholm, Sweden.ORCID iD: 0000-0002-8622-0308
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - BMC, Analytical Chemistry.ORCID iD: 0000-0002-4597-041x
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2021 (English)In: Limnology and Oceanography, ISSN 0024-3590, E-ISSN 1939-5590, Vol. 66, no 2, p. 496-509Article in journal (Refereed) Published
Abstract [en]

Autotrophic dissolved organic matter (DOM) is central to the carbon biogeochemistry of aquatic systems, and the full complexity of autotrophic DOM has not been extensively studied, particularly by high‐resolution mass spectrometry (HRMS). Terrestrial DOM tends to dominate HRMS studies in freshwaters due to the propensity of such compounds to ionize by negative mode electrospray, and possibly also because ionizable DOM produced by autotrophy is decreased to low steady‐state concentrations by heterotrophic bacteria. In this study, we investigated the character of DOM produced by the widespread cyanobacteria Microcystis aeruginosa using high‐pressure liquid chromatography—electrospray ionization—high‐resolution mass spectrometry. M. aeruginosa produced thousands of detectable compounds in axenic culture. These compounds were chromatographically resolved and the majority were assigned to aliphatic formulas with a broad polarity range. We found that the DOM produced by M. aeruginosa was highly susceptible to removal by heterotrophic freshwater bacteria, supporting the hypothesis that this autotroph‐derived organic material is highly labile and accordingly only seen at low concentrations in natural settings.

Place, publisher, year, edition, pages
Wiley John Wiley & Sons, 2021. Vol. 66, no 2, p. 496-509
National Category
Analytical Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-410263DOI: 10.1002/lno.11619ISI: 000577965400001OAI: oai:DiVA.org:uu-410263DiVA, id: diva2:1430179
Funder
Knut and Alice Wallenberg Foundation, 2013.0091The Royal Swedish Academy of Sciences, CR2019‐0060Swedish Research Council, 2015‐4870Swedish Research Council, 2017‐04422Swedish Research Council, 2018‐04618Available from: 2020-05-14 Created: 2020-05-14 Last updated: 2024-01-15Bibliographically approved
In thesis
1. Characterisation of natural dissolved organic matter with liquid chromatography and high resolution mass spectrometry
Open this publication in new window or tab >>Characterisation of natural dissolved organic matter with liquid chromatography and high resolution mass spectrometry
2020 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Dissolved organic matter (DOM) is one of the most heterogeneous and complex mixture on Earth. DOM plays a crucial role in biogeochemical processes on the global scale and it is essential to sustain and regulate the biological processes in aquatic ecosystems. DOM originates from a multitude of biological, physical and chemical transformations, leading to its phenomenal chemical diversity. In order to understand and predict its effect on the global carbon cycle, an intimate characterization at molecular level is necessary. The investigation of the extraordinary complexity of the DOM mixture represents a compelling challenge for analytical chemistry. The focus of this thesis was the development of methods for the characterization of DOM in natural waters. High resolution mass spectrometry (HRMS), was combined with high pressure liquid chromatography (HPLC) and electrospray ionization (ESI), to investigate the chemical diversity of DOM. The first study demonstrated that cutting-edge techniques (such as the Fourier-transform ion cyclotron resonance mass spectrometer - FTICR-MS), are not indispensable to disclose essential information on the DOM molecular composition, in fact the Orbitrap mass analyser is a suitable alternative for the analysis of complex natural mixtures. In the second study, the potential benefits offered by the online coupling of HPLC and HRMS instruments were explored, revealing significant advantages in terms of analysis time, achievable information and versatility of the method. The advantages of online separation were further confirmed in the third study, focused on the characterization of autochthonous labile DOM. Chromatographically resolved profiles emerged from the bulk-DOM, allowing the monitoring of labile autochthonous components in presence of heterotrophic bacteria. Despite the advantages achieved by the application of online separation, a strong limiting factor in DOM characterization is the ESI source, suitable only for the analysis of the DOM fraction susceptible to ionization. In the last study, the extent of the DOM material prone to ionization was estimated, revealing the occurrence of an extensive portion of the material resistant to routinely employed ESI approach. The full characterization of DOM is still an open challenge and the combination of multiple techniques is fundamental to unravel is extreme intricacy.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2020. p. 67
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 1948
Keywords
aquatic carbon cycle, dissolved organic matter, DOM, high resolution mass spectrometry, online liquid chromatography, organic matter characterization 
National Category
Analytical Chemistry
Research subject
Chemistry with specialization in Analytical Chemistry
Identifiers
urn:nbn:se:uu:diva-410266 (URN)978-91-513-0970-5 (ISBN)
Public defence
2020-09-04, B21, BMC, Husargatan 3, Uppsala, 09:15 (English)
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Supervisors
Available from: 2020-06-11 Created: 2020-05-14 Last updated: 2020-12-23

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Patriarca, ClaudiaGarcia, Sarahi LBergquist, JonasBertilsson, StefanSjöberg, Per J. R.Tranvik, LarsHawkes, Jeffrey A.

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Patriarca, ClaudiaSedano Núñez, Vicente T.Garcia, Sarahi LBergquist, JonasBertilsson, StefanSjöberg, Per J. R.Tranvik, LarsHawkes, Jeffrey A.
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Analytical ChemistryMolecular EvolutionScience for Life Laboratory, SciLifeLabLimnology
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