| 1. |
- Hawkes, Jeffrey A., et al.
(författare)
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An international laboratory comparison of dissolved organic matter composition by high resolution mass spectrometry : Are we getting the same answer?
- 2020
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Ingår i: Limnology and Oceanography. - : Wiley. - 1541-5856. ; 18:6, s. 235-258
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Tidskriftsartikel (refereegranskat)abstract
- High-resolution mass spectrometry (HRMS) has become a vital tool for dissolved organic matter (DOM) characterization. The upward trend in HRMS analysis of DOM presents challenges in data comparison and interpretation among laboratories operating instruments with differing performance and user operating conditions. It is therefore essential that the community establishes metric ranges and compositional trends for data comparison with reference samples so that data can be robustly compared among research groups. To this end, four identically prepared DOM samples were each measured by 16 laboratories, using 17 commercially purchased instruments, using positive-ion and negative-ion mode electrospray ionization (ESI) HRMS analyses. The instruments identified similar to 1000 common ions in both negative- and positive-ion modes over a wide range of m/z values and chemical space, as determined by van Krevelen diagrams. Calculated metrics of abundance-weighted average indices (H/C, O/C, aromaticity and m/z) of the commonly detected ions showed that hydrogen saturation and aromaticity were consistent for each reference sample across the instruments, while average mass and oxygenation were more affected by differences in instrument type and settings. In this paper we present 32 metric values for future benchmarking. The metric values were obtained for the four different parameters from four samples in two ionization modes and can be used in future work to evaluate the performance of HRMS instruments.
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| 2. |
- Attermeyer, Katrin, et al.
(författare)
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Organic Carbon Processing During Transport Through Boreal Inland Waters : Particles as Important Sites
- 2018
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Ingår i: Journal of Geophysical Research - Biogeosciences. - 2169-8953 .- 2169-8961. ; 123:8, s. 2412-2428
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Tidskriftsartikel (refereegranskat)abstract
- The degradation and transformation of organic carbon (C) in inland waters result in significant CO2 emissions from inland waters. Even though most of the C in inland waters occurs as dissolved organic carbon (DOC), studies on particulate organic carbon (POC) and how it influences the overall reactivity of organic C in transport are still scarce. We sampled 30 aquatic ecosystems following an aquatic continuum including peat surface waters, streams, rivers, and lakes. We report DOC and POC degradation rates, relate degradation patterns to environmental data across these systems, and present qualitative changes in dissolved organic matter and particulate organic matter during degradation. Microbial degradation rates of POC were approximately 15 times higher compared to degradation of DOC, with POC half-lives of only 17 +/- 3 (mean +/- SE) days across all sampled aquatic ecosystems. Rapid POC decay was accompanied by a shift in particulate C: N ratios, whereas dissolved organic matter composition did not change at the time scale of incubations. The faster degradation of the POC implies a constant replenishment to sustain natural POC concentrations. We suggest that degradation of organic matter transported through the inland water continuum might occur to a large extent via transition of DOC into more rapidly cycling POC in nature, for example, triggered by light. In this way, particles would be a dominant pool of organic C processing across the boreal aquatic continuum, partially sustained by replenishment via flocculation of DOC.
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| 3. |
- Berggren, Martin, et al.
(författare)
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Unified understanding of intrinsic and extrinsic controls of dissolved organic carbon reactivity in aquatic ecosystems
- 2022
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Ingår i: Ecology. - : Wiley. - 0012-9658 .- 1939-9170. ; 103:9
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Tidskriftsartikel (refereegranskat)abstract
- Despite our growing understanding of the global carbon cycle, scientific consensus on the drivers and mechanisms that control dissolved organic carbon (DOC) turnover in aquatic systems is lacking, hampered by the mismatch between research that approaches DOC reactivity from either intrinsic (inherent chemical properties) or extrinsic (environmental context) perspectives. Here we propose a conceptual view of DOC reactivity in which the combination of intrinsic and extrinsic factors controls turnover rates and determines which reactions will occur. We review three major types of reactions (biological, photochemical, and flocculation) from an intrinsic chemical perspective and further define the environmental features that modulate the expression of chemically inherent reactivity potential. Finally, we propose hypotheses of how extrinsic and intrinsic factors together shape patterns in DOC turnover across the land-to-ocean continuum, underscoring that there is no intrinsic DOC reactivity without environmental context. By acknowledging the intrinsic–extrinsic control duality, our framework intends to foster improved modeling of DOC reactivity and its impact on ecosystem services.
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| 4. |
- Capo, Eric, et al.
(författare)
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Expression Levels of hgcAB Genes and Mercury Availability Jointly Explain Methylmercury Formation in Stratified Brackish Waters
- 2022
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Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 56:18, s. 13119-13130
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Tidskriftsartikel (refereegranskat)abstract
- Neurotoxic methylmercury (MeHg) is formed by microbial methylation of inorganic divalent Hg (Hg-II) and constitutes severe environmental and human health risks. The methylation is enabled by hgcA and hgcB genes, but it is not know nif the associated molecular-level processes are rate-limiting or enable accurate prediction of MeHg formation in nature. In this study, we investigated the relationships between hgc genes and MeHg across redox-stratified water columns in the brackish Baltic Sea. We showed, for the first time, that hgc transcript abundance and the concentration of dissolved Hg-II-sulfide species were strong predictors of both the Hg-II methylation rate and MeHg concentration, implying their roles as principal joint drivers of MeHg formation in these systems. Additionally, we characterized the metabolic capacities of hgc(+) microorganisms by reconstructing their genomes from metagenomes (i.e., hgc(+) MAGs), which highlighted the versatility of putative Hg-II methylators in the water column of the Baltic Sea. In establishing relationships between hgc transcripts and the Hg-II methylation rate, we advance the fundamental understanding of mechanistic principles governing MeHg formation in nature and enable refined predictions of MeHg levels in coastal seas in response to the accelerating spread of oxygen-deficientzones.
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| 5. |
- Catalan, Nuria, et al.
(författare)
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The relevance of environment vs. composition on dissolved organic matter degradation in freshwaters
- 2021
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Ingår i: Limnology and Oceanography. - : John Wiley & Sons. - 0024-3590 .- 1939-5590. ; 66:2, s. 306-320
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Tidskriftsartikel (refereegranskat)abstract
- Dissolved organic matter (DOM) composition exerts a direct control on its degradation and subsequent persistence in aquatic ecosystems. Yet, under certain conditions, the degradation patterns of DOM cannot be solely explained by its composition, highlighting the relevance of environmental conditions for DOM degradation. Here, we experimentally assessed the relative influence of composition vs. environment on DOM degradation by performing degradation bioassays using three contrasting DOM sources inoculated with a standardized bacterial inoculum under five distinct environments. The DOM degradation kinetics modeled using reactivity continuum models showed that composition was more important than environment in determining the bulk DOM decay patterns. Changes in DOM composition resulted from the interaction between DOM source and environment. The role of environment was stronger on shaping the bacterial community composition, but the intrinsic nature of the DOM source exerted stronger control on the DOM degradation function.
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| 6. |
- Craig, Alexander J., et al.
(författare)
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Antimicrobial Peptides Incorporating Halogenated Marine-Derived Amino Acid Substituents
- 2023
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Ingår i: ACS Medicinal Chemistry Letters. - : American Chemical Society (ACS). - 1948-5875. ; 14:6, s. 802-809
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Tidskriftsartikel (refereegranskat)abstract
- Small synthetic mimics of cationic antimicrobial peptides represent a promising class of compounds with leads in clinical development for the treatment of persistent microbial infections. The activity and selectivity of these compounds rely on a balance between hydrophobic and cationic components, and here, we explore the activity of 19 linear cationic tripeptides against five different pathogenic bacteria and fungi, including clinical isolates. The compounds incorporated modified hydrophobic amino acids inspired by motifs often found in bioactive marine secondary metabolites in combination with different cationic residues to probe the possibility of generating active compounds with improved safety profiles. Several of the compounds displayed high activity (low mu M concentrations), comparable with the positive controls AMC-109, amoxicillin, and amphotericin B. A higher activity was observed against the fungal strains, and a low in vitro off-target toxicity was observed against erythrocytes and HeLa cells, thereby illustrating effective means for tuning the activity and selectivity of short antimicrobial peptides.
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| 7. |
- Craig, Alexander J., et al.
(författare)
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Preparation of Simple Bicyclic Carboxylate-Rich Alicyclic Molecules for the Investigation of Dissolved Organic Matter
- 2024
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Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 58:16, s. 7078-7086
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Tidskriftsartikel (refereegranskat)abstract
- Dissolved organic matter (DOM) is a vast and complex chemical mixture that plays a key role in the mediation of the global carbon cycle. Fundamental understanding of the source and fate of oceanic organic matter is obscured due to poor definition of the key molecular contributors to DOM, which limits accurate sample analysis and prediction of the Earth's carbon cycle. Previous work has attempted to define the components of the DOM through a variety of chromatographic and spectral techniques. However, modern preparative and analytical methods have not isolated or unambiguously identified molecules from DOM. Therefore, previously proposed structures are based solely on the mixture's aggregate properties and do not accurately describe any true individual molecular component. In addition to this, there is a lack of appropriate analogues of the individual chemical classes within DOM, limiting the scope of experiments that probe the physical, chemical, and biological contributions from each class. To address these problems, we synthesized a series of analogues of carboxylate-rich alicyclic molecules (CRAM), a molecular class hypothesized to exist as a major contributor to DOM. Key analytical features of the synthetic CRAMs were consistent with marine DOM, supporting their suitability as chemical substitutes for CRAM. This new approach provides access to a molecular toolkit that will enable previously inaccessible experiments to test many unproven hypotheses surrounding the ever-enigmatic DOM.
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| 8. |
- Duncan, Kyle D., et al.
(författare)
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Membrane Sampling Separates Naphthenic Acids from Biogenic Dissolved Organic Matter for Direct Analysis by Mass Spectrometry
- 2022
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Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 56:5, s. 3096-3105
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Tidskriftsartikel (refereegranskat)abstract
- Oil sands process waters can release toxic naphthenic acids (NAs) into aquatic environments. Analytical techniques for NAs are challenged by sample complexity and interference from naturally occurring dissolved organic matter (DOM). Herein, we report the use of a poly(dimethylsiloxane) (PDMS) polymer membrane for the on-line separation of NAs from DOM and use direct infusion electrospray ionization mass spectrometry to yield meaningful qualitative and quantitative information with minimal sample cleanup. We compare the composition of membrane-permeable species from natural waters fortified with a commercial NA mixture to those derived from weak anion exchange solid-phase extraction (SPE) using high-resolution mass spectrometry. The results show that SPE retains a wide range of carboxylic acids, including biogenic DOM, while permeation through PDMS was selective for petrogenic classically defined NAs (CnH2n+zO2). A series of model compounds (log K-ow similar to 1-7) were used to characterize the perm-selectivity and reveal the separation is based on hydrophobicity. This convenient sample cleanup method is selective for the O-2 class of NAs and can be used prior to conventional analysis or as an on-line analytical strategy when coupled directly to mass spectrometry.
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| 9. |
- Durall de la Fuente, Claudia, et al.
(författare)
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Production of succinate by engineered strains of Synechocystis PCC 6803 overexpressing phosphoenolpyruvate carboxylase and a glyoxylate shunt
- 2021
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Ingår i: Microbial Cell Factories. - : BioMed Central (BMC). - 1475-2859. ; 20
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Tidskriftsartikel (refereegranskat)abstract
- Background: Cyanobacteria are promising hosts for the production of various industrially important compounds such as succinate. This study focuses on introduction of the glyoxylate shunt, which is naturally present in only a few cyanobacteria, into Synechocystis PCC 6803. In order to test its impact on cell metabolism, engineered strains were evaluated for succinate accumulation under conditions of light, darkness and anoxic darkness. Each condition was complemented by treatments with 2-thenoyltrifluoroacetone, an inhibitor of succinate dehydrogenase enzyme, and acetate, both in nitrogen replete and deplete medium.Results: We were able to introduce genes encoding the glyoxylate shunt, aceA and aceB, encoding isocitrate lyase and malate synthase respectively, into a strain of Synechocystis PCC 6803 engineered to overexpress phosphoenolpyruvate carboxylase. Our results show that complete expression of the glyoxylate shunt results in higher extracellular succinate accumulation compared to the wild type control strain after incubation of cells in darkness and anoxic darkness in the presence of nitrate. Addition of the inhibitor 2-thenoyltrifluoroacetone increased succinate titers in all the conditions tested when nitrate was available. Addition of acetate in the presence of the inhibitor further increased the succinate accumulation, resulting in high levels when phosphoenolpyruvate carboxylase was overexpressed, compared to control strain. However, the highest succinate titer was obtained after dark incubation of an engineered strain with a partial glyoxylate shunt overexpressing isocitrate lyase in addition to phosphoenolpyruvate carboxylase, with only 2-thenoyltrifluoroacetone supplementation to the medium.Conclusions: Heterologous expression of the glyoxylate shunt with its central link to the tricarboxylic acid cycle (TCA) for acetate assimilation provides insight on the coordination of the carbon metabolism in the cell. Phosphoenolpyruvate carboxylase plays an important role in directing carbon flux towards the TCA cycle.
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| 10. |
- Einarsdóttir, Karólina, 1980-
(författare)
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Mire Aeration & Particles Experiment : Dataset from the study: Particles and aeration at mire-stream interfaces cause selective removal and modification of dissolved organic matter. Article accepted by AGU-JGR-Biogeosciences
- 2020
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Annan publikationabstract
- The dataset contains physio-chemical data from an experiment that aimed to answer how aeration of anoxic mire water, and suspended particles, may impacts dissolved organic matter in both quality and quantity. The experimental data gives idea how physio-chemical parameters may change upon aeration, e.g., at soil-water interfaces or when anoxic mire water merges into a stream and the water is mixed with the atmosphere. In addition, the importance of suspended particles that are found in the mire water was also examined. The dataset comprises measured concentrations of dissolved organic carbon (DOC), inorganic carbon (IC), particulate organic carbon (POC) and particulate nitrogen (PN), dissolved iron (DFe, divided in ferrous (Fe (II)) and ferric (Fe(III)) forms), dissolved oxygen, temperature, chemical composition of DOM (intensity of formulas CHO) divided in three fractions depending on hydrophobicity, and intensity of absorbance of 254nm. The study was conducted in September 2017 and the samples come from a sloping mire that drains into small headwater-stream and is located in a boreal forest of Mid-Sweden. The samples were anoxic and sampled for all parameters in a nitrogen aired glovebox prior the experiment start, half of the samples were aerated, and half of the aerated and half of the anoxic samples contained particles from the mire while the other half was filtered through GF/F filter. After aeration, samples for DFe species and IC were taken from aerated samples. Oxygen was monitored the whole time. The experiment went on for five days and then all parameters were measured again.
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