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Identifying controls of adsorption capacity on the molecular composition of dissolved organic matter using a multi-analytical approach
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Biologiska sektionen, Institutionen för ekologi och genetik, Limnologi.ORCID-id: 0000-0003-1988-3870
National High Magnetic Field Laboratory Geochemistry Group and Department of Earth, Ocean, and Atmospheric Science, Florida State University, Tallahassee, Florida.ORCID-id: 0000-0002-7348-4814
Uppsala universitet, Teknisk-naturvetenskapliga vetenskapsområdet, Kemiska sektionen, Institutionen för kemi - BMC.ORCID-id: 0000-0002-8165-5863
National High Magnetic Field Laboratory, Florida State University, 1800 East Paul Dirac Drive, Tallahassee, Florida 32310-4005, USA.ORCID-id: 0000-0001-7213-521X
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(Engelska)Manuskript (preprint) (Övrigt vetenskapligt)
Abstract [en]

Dissolved organic matter (DOM) composition in terrestrial and aquatic ecosystems is controlled by various physical and biogeochemical processes, including adsorption to mineral particles. Advancing our knowledge of DOM-mineral interactions is crucial for assessing long-term carbon storage in ecosystems. Considerable efforts have been made to characterize how DOM-mineral interactions influence DOM composition, yet the impact of adsorption extent on shaping DOM composition remains poorly understood. In this study, we investigate how DOM composition changes across a gradient of adsorption capacity by studying adsorption interactions between five widely different DOM sources originating from terrestrial and aquatic ecosystems and five minerals that have largely distinct characteristics. We also used a multi-analytical approach for DOM characterization by combining fluorescence analysis, mass spectrometry (FT-ICR MS) and 1H NMR, allowing us to gain a more comprehensive overview of changes in DOM chemical composition due to adsorption. By including 1H NMR analysis, we captured changes to carbohydrate-like compounds, which are potentially energy-rich for microbial uptake and respiration. We found that strong adsorption interactions preferentially removed more oxygen-rich DOM compounds with higher aromatic and polyphenolic fractions, while weak adsorption was less selective and removed a broader range of DOM fractions. Selective removal for strong DOM-mineral interactions led to the enrichment of more aliphatic, protein-like structures and carbohydrates in the remaining DOM pool. The findings of this study have important ecological implications in terms of energy availability for microorganisms and predicting carbon sequestration in terrestrial ecosystems and inland waters, where agricultural, mining, and forestry activities increase mineral particle presence and enhance DOM-mineral interactions.

Nyckelord [en]
DOM-mineral interactions, adsorption, DOM compositional changes, fluorescence, mass spectrometry, 1H NMR
Nationell ämneskategori
Analytisk kemi Organisk kemi Miljövetenskap Oceanografi, hydrologi och vattenresurser Biologi
Identifikatorer
URN: urn:nbn:se:uu:diva-554724OAI: oai:DiVA.org:uu-554724DiVA, id: diva2:1952427
Tillgänglig från: 2025-04-15 Skapad: 2025-04-15 Senast uppdaterad: 2025-05-06
Ingår i avhandling
1. Adsorption and biological degradation of dissolved organic matter in terrestrial and aquatic ecosystems
Öppna denna publikation i ny flik eller fönster >>Adsorption and biological degradation of dissolved organic matter in terrestrial and aquatic ecosystems
2025 (Engelska)Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)
Abstract [en]

Dissolved organic matter (DOM) is a complex mixture of organic compounds found across the biosphere. DOM concentration and composition are highly dynamic because of various transformation processes, such as microbial and photochemical degradation and adsorption to mineral particles. These processes are essential for carbon cycling across ecosystems and for water quality. Adsorption is important for DOM cycling, but its role in changing DOM composition and biological reactivity is rarely studied together. Extrinsic controls induced by water residence time can also impact DOM both spatially and temporally, yet these dynamics are poorly known. This thesis aims to fill these knowledge gaps in four studies. In the first study, DOM treatability and biodegradability across lake Mälaren in Sweden were investigated at six time points. The findings show that water residence time (WRT) plays a key role in shaping the composition of DOM. As WRT increases, DOM concentration and composition resist seasonality-driven temporal variations and gradually shift from terrestrial to aquatic origin, which enhances its treatability for drinking water. In the three following studies, batch experiments were sequentially performed to investigate adsorption controls on DOM composition and biodegradability across a range of mineral types and DOM sources from terrestrial and aquatic environments. The experiments (i) quantify adsorption capacities, (ii) evaluate DOM compositional changes due to adsorption using a multi-analytical approach incorporating fluorescence spectroscopy, mass spectrometry, and 1H NMR, and (iii) assess the biodegradability of the remaining DOM pool. The outcomes highlight that the adsorption capacity depends on the DOM sources, characteristics of mineral surfaces, and water chemistry. Strong adsorption interactions preferentially remove oxygen-rich, aromatic DOM, while weak interactions tend to target more diverse compounds. Moreover, DOM-mineral interactions have varying effects on biodegradability, ranging from strong to moderate and no enhancement after adsorption. The multi-analytical approach improves DOM characterization by reducing individual method biases. Notably, ¹H NMR effectively detects carbohydrate fractions, which are often overlooked by other methods. The thesis has important implications for descriptions of carbon dynamics in terrestrial and aquatic ecosystems, where agricultural, mining, and forestry increase mineral presence and enhance organo-mineral interactions.

Ort, förlag, år, upplaga, sidor
Uppsala: Acta Universitatis Upsaliensis, 2025. s. 58
Serie
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 2544
Nyckelord
dissolved organic matter, DOM characterization, adsorption, minerals, terrestrial, aquatic, ultrahigh-resolution mass spectrometry, FT-ICR MS, 1H NMR, soil organic matter, carbon cycling
Nationell ämneskategori
Naturvetenskap
Forskningsämne
Biologi med inriktning mot limnologi
Identifikatorer
urn:nbn:se:uu:diva-554726 (URN)978-91-513-2489-0 (ISBN)
Disputation
2025-06-12, Friessalen, EBC, Norbyvägen 16, Uppsala, 13:00 (Engelska)
Opponent
Handledare
Tillgänglig från: 2025-05-20 Skapad: 2025-04-15 Senast uppdaterad: 2025-05-20

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Av författaren/redaktören
Abbasi, MonaKellerman, AnneXiong, RuishengMcKenna, AmyKothawala, Dolly
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LimnologiInstitutionen för kemi - BMC
Analytisk kemiOrganisk kemiMiljövetenskapOceanografi, hydrologi och vattenresurserBiologi

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