| 1. |
- Allesson, Lina, et al.
(författare)
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The role of photomineralization for CO2 emissions in boreal lakes along a gradient of dissolved organic matter
- 2021
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Ingår i: Limnology and Oceanography. - : John Wiley & Sons. - 0024-3590 .- 1939-5590. ; 66:1, s. 158-170
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Tidskriftsartikel (refereegranskat)abstract
- Many boreal lakes are experiencing an increase in concentrations of terrestrially derived dissolved organic matter (DOM)-a process commonly labeled "browning." Browning affects microbial and photochemical mineralization of DOM, and causes increased light attenuation and hence reduced photosynthesis. Consequently, browning regulates lake heterotrophy and net CO2-efflux to the atmosphere. Climate and environmental change makes ecological forecasting and global carbon cycle modeling increasingly important. A proper understanding of the magnitude and relative contribution from CO2-generating processes for lakes ranging in dissolve organic carbon (DOC) concentrations is therefore crucial for constraining models and forecasts. Here, we aim to study the relative contribution of photomineralization to total CO(2)production in 70 Scandinavian lakes along an ecosystem gradient of DOC concentration. We combined spectral data from the lakes with regression estimates between optical parameters and wavelength specific photochemical reactivity to estimate rates of photochemical DOC mineralization. Further, we estimated total in-lake CO2-production and efflux from lake chemical and physical data. Photochemical mineralization corresponded on average to 9% +/- 1% of the total CO2-evasion, with the highest contribution in clear lakes. The calculated relative contribution of photochemical mineralization to total in-lake CO2-production was about 3% +/- 0.2% in all lakes. Although lakes differed substantially in color, depth-integrated photomineralization estimates were similar in all lakes, regardless of DOC concentrations. DOC concentrations were positively related to CO2-efflux and total in-lake CO2-production but negatively related to primary production. We conclude that enhanced rates of photochemical mineralization will be a minor contributor to increased heterotrophy under increased browning.
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| 2. |
- Koehler, Birgit, 1980-, et al.
(författare)
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Inter-laboratory differences in the apparent quantum yield for the photochemical production of dissolved inorganic carbon in inland waters and implications for photochemical rate modeling
- 2022
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Ingår i: Limnology and Oceanography. - : John Wiley & Sons. - 1541-5856. ; 20:6, s. 320-337
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Tidskriftsartikel (refereegranskat)abstract
- Solar radiation initiates photochemical oxidation of dissolved organic carbon (DOC) to dissolved inorganic carbon (DIC) in inland waters, contributing to their carbon dioxide emissions to the atmosphere. Models can determine photochemical DIC production over large spatiotemporal scales and assess its role in aquatic C cycling. The apparent quantum yield (AQY) spectrum for photochemical DIC production, defined as mol DIC produced per mol chromophoric dissolved organic matter-absorbed photons, is a critical model parameter. In previous studies, the principle for the determination of AQY spectra is the same but methodological specifics differ, and the extent to which these differences influence AQY spectra and simulated aquatic DIC photoproduction is unclear. Here, four laboratories determined AQY spectra from water samples of eight inland waters that are situated in Alaska, Finland, and Sweden and span a nearly 10-fold range in DOM absorption coefficients. All AQY values fell within the range previously reported for inland waters. The inter-laboratory coefficient of variation (CV) for wavelength-integrated AQY spectra (300-450 nm) averaged 38% +/- 3% SE, and the inter-water CV averaged 63% +/- 1%. The inter-laboratory CV for simulated photochemical DIC production (conducted for the five Swedish lakes) averaged 49% +/- 12%, and the inter-water CV averaged 77% +/- 10%. This uncertainty is not surprising given the complexities and methodological choices involved in determining DIC AQY spectra and needs to be considered when applying photochemical rate modeling. Thus, we also highlight current methodological limitations and suggest future improvements for DIC AQY determination to reduce inter-laboratory uncertainty.
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| 3. |
- Koehler, Birgit, 1980-, et al.
(författare)
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Simulation of photoreactive transients and of photochemical transformation of organic pollutants in sunlit boreal lakes across 14 degrees of latitude : A photochemical mapping of Sweden
- 2018
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Ingår i: Water Research. - : Elsevier. - 0043-1354 .- 1879-2448. ; 129, s. 94-104
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Tidskriftsartikel (refereegranskat)abstract
- Lake water constituents, such as chromophoric dissolved organic matter (CDOM) and nitrate, absorb sunlight which induces an array of photochemical reactions. Although these reactions are a substantial driver of pollutant degradation in lakes they are insufficiently understood, in particular on large scales. Here, we provide for the first time comprehensive photochemical maps covering a large geographic region. Using photochemical kinetics modeling for 1048 lakes across Sweden we simulated the steady-state concentrations of four photoreactive transient species, which are continuously produced and consumed in sunlit lake waters. We then simulated the transient-induced photochemical transformation of organic pollutants, to gain insight into the relevance of the different photoreaction pathways. We found that boreal lakes were often unfavorable environments for photoreactions mediated by hydroxyl radicals ([rad]OH) and carbonate radical anions (CO3−[rad]), while photoreactions mediated by CDOM triplet states (3CDOM*) and, to a lesser extent, singlet oxygen (1O2) were the most prevalent. These conditions promote the photodegradation of phenols, which are used as plastic, medical drug and herbicide precursors. When CDOM concentrations increase, as is currently commonly the case in boreal areas such as Sweden,3CDOM* will also increase, promoting its importance in photochemical pathways even more.
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| 4. |
- Koehler, Birgit, 1980-, et al.
(författare)
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Sunlight-induced carbon dioxide emissions from inland waters
- 2014
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Ingår i: Global Biogeochemical Cycles. - 0886-6236 .- 1944-9224. ; 28:7, s. 696-711
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Tidskriftsartikel (refereegranskat)abstract
- The emissions of carbon dioxide (CO2) from inland waters are substantial on a global scale. Yet, the fundamental question remains open which proportion of these CO2 emissions is induced by sunlight via photochemical mineralization of dissolved organic carbon (DOC), rather than by microbial respiration during DOC decomposition. Also, it is unknown on larger spatial and temporal scales how photochemical mineralization compares to other C fluxes in the inland water C cycle. We combined field and laboratory data with atmospheric radiative transfer modeling to parameterize a photochemical rate model for each day of the year 2009, for 1086 lakes situated between latitudes from 55 to 69°N in Sweden. The sunlight-induced production of dissolved inorganic carbon (DIC) averaged 3.8 ± 0.04 g C m-2 yr-1, which is a flux comparable in size to the organic carbon burial in the lake sediments. Countrywide, 151 ± 1 kt C yr-1 was produced by photochemical mineralization, corresponding to about 12% of total annual mean CO2 emissions from Swedish lakes. With a median depth of 3.2 m, the lakes were generally deep enough that incoming, photochemically active photons were absorbed in the water column. This resulted in a linear positive relationship between DIC photoproduction and the incoming photon flux, which correspond to the absorbed photons. Therefore, the slope of the regression line represents the wavelength- and depth-integrated apparent quantum yield of DIC photoproduction. We used this relationship to obtain a first estimate of DIC photoproduction in lakes and reservoirs worldwide. Global DIC photoproduction amounted to 13 and 35 Mt C yr-1 under overcast and clear sky, respectively. Consequently, these directly sunlight-induced CO2 emissions contribute up to about one tenth to the global CO2 emissions from lakes and reservoirs, corroborating that microbial respiration contributes a substantially larger share than formerly thought, and generate annual C fluxes similar in magnitude to the C burial in natural lake sediments worldwide.
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| 5. |
- Mostovaya, Alina, 1985-, et al.
(författare)
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Emergence of the Reactivity Continuum of Organic Matter from Kinetics of a Multitude of Individual Molecular Constituents
- 2017
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Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 51:20, s. 11571-11579
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Tidskriftsartikel (refereegranskat)abstract
- The reactivity continuum (RC) model is a powerful statistical approach for describing the apparent kinetics of bulk organic matter (OM) decomposition. Here, we used ultrahigh resolution mass spectrometry data to evaluate the main premise of the RC model, namely that there is a continuous spectrum of reactivity within bulk OM, where each individual reactive type undergoes exponential decay. We performed a 120 day OM decomposition experiment on lake water, with an untreated control and a treatment preexposed to UV light, and described the loss of bulk dissolved organic carbon with RC modeling. The behavior of individual molecular formulas was described by fitting the single exponential model to the change in peak intensities over time. The range of the empirically derived apparent exponential decay coefficients (kexp) was indeed continuous. The character of the corresponding distribution, however, differed from the conceptual expectations, due to the effects of intrinsic averaging, overlaps in formula-specific loss and formation rates, and the limitation of the RC model to include apparently accumulating compounds in the analysis. Despite these limitations, both the RC model-simulated and empirical (mass spectrometry-derived) distributions of kexp captured the effects of preexposure to UV light. Overall, we present experimental evidence that the reactivity continuum within bulk OM emerges from a range of reactivity of numerous individual components. This constitutes direct empirical support for the major assumption behind the RC model of the natural OM decomposition.
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| 6. |
- Sobek, Sebastian, et al.
(författare)
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Temperature dependence of apparent respiratory quotients and oxygen penetration depth in contrasting lake sediments
- 2017
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Ingår i: Journal of Geophysical Research - Biogeosciences. - Washington : American Geophysical Union (AGU). - 2169-8953 .- 2169-8961. ; 122:11, s. 3076-3087
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Tidskriftsartikel (refereegranskat)abstract
- Lake sediments constitute an important compartment in the carbon cycle of lakes, by burying carbon over geological timescales and by production and emission of greenhouse gases. The degradation of organic carbon (OC) in lake sediments is linked to both temperature and oxygen (O-2), but the interactive nature of this regulation has not been studied in lake sediments in a quantitative way. We present the first systematic investigation of the effects of temperature on the apparent respiratory quotient (RQ, i.e., the molar ratio between carbon dioxide (CO2) production and O-2 consumption) in two contrasting lake sediments. Laboratory incubations of sediment cores of a humic lake and an eutrophic lake across a 1-21 degrees C temperature gradient over 157days revealed that both CO2 production and O-2 consumption were positively, exponentially, and similarly dependent on temperature. The apparent RQ differed significantly between the lake sediments (0.630.26 and 0.990.28 in the humic and the eutrophic lake, respectively; meanSD) and was significantly and positively related to temperature. The O-2 penetration depth into the sediment varied by a factor of 2 over the 1-21 degrees C temperature range and was significantly, negatively, and similarly related to temperature in both lake sediments. Accordingly, increasing temperature may influence the overall extent of OC degradation in lake sediments by limiting O-2 supply to aerobic microbial respiration to the topmost sediment layer, resulting in a concomitant shift to less effective anaerobic degradation pathways. This suggests that temperature may represent a key controlling factor of the OC burial efficiency in lake sediments.
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| 7. |
- Veldkamp, Edzo, et al.
(författare)
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Indications of nitrogen-limited methane uptake in tropical forest soils
- 2013
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Ingår i: Biogeosciences. - : Copernicus GmbH. - 1726-4170 .- 1726-4189. ; 10:8, s. 5367-5379
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Tidskriftsartikel (refereegranskat)abstract
- Abstract: It is estimated that tropical forest soils contribute 6.2 Tg yr(-1) (28 %) to global methane (CH4) uptake, which is large enough to alter CH4 accumulation in the atmosphere if significant changes would occur to this sink. Elevated deposition of inorganic nitrogen (N) to temperate forest ecosystems has been shown to reduce CH4 uptake in forest soils, but almost no information exists from tropical forest soils even though projections show that N deposition will increase substantially in tropical regions. Here we report the results from two long-term, ecosystem-scale experiments in which we assessed the impact of chronic N addition on soil CH4 fluxes from two old-growth forests in Panama: (1) a lowland, moist (2.7 m yr(-1) rainfall) forest on clayey Cambisol and Nitisol soils with controls and N-addition plots for 9-12yr, and (2) a montane, wet (5.5 m yr(-1) rainfall) forest on a sandy loam Andosol soil with controls and N-addition plots for 1-4 yr. We measured soil CH4 fluxes for 4 yr (2006-2009) in four replicate plots (40 m x 40 m each) per treatment using vented static chambers (four chambers per plot). CH4 fluxes from the lowland control plots and the montane control plots did not differ from their respective N-addition plots. In the lowland forest, chronic N addition did not lead to inhibition of CH4 uptake; instead, a negative correlation of CH4 fluxes with nitrate (NO3-) concentrations in the mineral soil suggests that increased NO3- levels in N-addition plots had stimulated CH4 consumption and/or reduced CH4 production. In the montane forest, chronic N addition also showed negative correlation of CH4 fluxes with ammonium concentrations in the organic layer, which suggests that CH4 consumption was N limited. We propose the following reasons why such N-stimulated CH4 consumption did not lead to statistically significant CH4 uptake: (1) for the lowland forest, this was caused by limitation of CH4 diffusion from the atmosphere into the clayey soils, particularly during the wet season, as indicated by the strong positive correlations between CH4 fluxes and water-filled pore space (WFPS); (2) for the montane forest, this was caused by the high WFPS in the mineral soil throughout the year, which may not only limit CH4 diffusion from the atmosphere into the soil but also favour CH4 production; and (3) both forest soils showed large spatial and temporal variations of CH4 fluxes. We conclude that in these extremely different tropical forest ecosystems there were indications of N limitation on CH4 uptake. Based on these findings, it is unlikely that elevated N deposition on tropical forest soils will lead to a rapid reduction of CH4 uptake.
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| 8. |
- Vione, Davide, et al.
(författare)
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Modelled phototransformation kinetics of the antibiotic sulfadiazine in organic matter-rich lakes
- 2018
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Ingår i: Science of the Total Environment. - : ELSEVIER SCIENCE BV. - 0048-9697 .- 1879-1026. ; 645, s. 1465-1473
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Tidskriftsartikel (refereegranskat)abstract
- Xenobiotic compounds are commonly detected in inland waters. Sunlight-induced photochemical reactions contribute to xenobiotic degradation, but the role of different photoreactions on large geographic scales remains poorly understood. Here, we used a combination of photochemical modelling and large-scale field data from 1020 lakes across Sweden to elucidate the photodegradation kinetics of the commonly used antibiotic sulfadiazine (SDZ) in organic matter-rich lakes. SDZ occurs in two forms, namely acidic HSDZ (pK(a) = 6.5) and basic/deprotonated SDZ . Both species are oxidised fast by the photogenerated triplet states of natural organic matter ((NOM)-N-3*). However, they also undergo efficient back reactions because the partially oxidised HSDZ (and SDZ(-) to a larger extent) can be reduced back to the initial compounds by the phenolic moieties contained in NOM. Typical lakes in Sweden are rich in NOM and have low pH, with the consequence that SDZ photochemistry would be dominated by HSDZ. Our simulation results showed that SDZ photodegradation kinetics in Swedish lakes would become significantly slower with increasing water depth and pH, while it depended little on latitude, which affects irradiance, or on organic matter content. As a consequence, SDZ would be particularly persistent in lakewater in some densely populated areas with relatively deep and high-pH lakes such as, most notably, the Stockholm region. Here the surface waters could be more heavily contaminated by pharmaceuticals compared to the scarcely populated regions in the centre-north of the country, where lakewater could otherwise promote an efficient photodegradation of SDZ.
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