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Tree growth in boreal forests is driven by ectomycorrhizal fungal mobilisation of organic nitrogen and mineral nutrients in soils with discrete organic and mineral horizons. However, there are no studies of how ectomycorrhizal mineral weathering and organic nitrogen mobilisation processes are integrated across the soil profile. We studied effects of organic matter (OM) availability on ectomycorrhizal functioning by altering the proportions of natural organic and mineral soil in reconstructed podzol profiles containing Pinus sylvestris plants, using 13 CO 2 pulse labelling, patterns of naturally occurring stable isotopes ( 26 Mg and 15 N) and high-throughput DNA sequencing of fungal amplicons. Reduction in OM resulted in nitrogen limitation of plant growth and decreased allocation of photosynthetically derived carbon and mycelial growth in mineral horizons. Fractionation patterns of 26 Mg indicated that magnesium mobilisation and uptake occurred primarily in the deeper mineral horizon and was driven by carbon allocation to ectomycorrhizal mycelium. In this horizon, relative abundance of ectomycorrhizal fungi, carbon allocation and base cation mobilisation all increased with increased OM availability. Allocation of carbon through ectomycorrhizal fungi integrates organic nitrogen mobilisation and mineral weathering across soil horizons, improving the efficiency of plant nutrient acquisition. Our findings have fundamental implications for sustainable forest management and belowground carbon sequestration., (© 2023 The Authors. New Phytologist © 2023 New Phytologist Foundation.)

Persistent, mobile, and toxic (PMT) substances have recently garnered increased attention by environmental researchers, the water sector and environmental protection agencies. In this study, acute and chronic species sensitivity distributions (SSDs) were retrieved from literature data for previously quantified contaminants of emerging concern (CECs) in Swedish surface waters (n = 92) and risk quotients (RQ) were calculated. To better understand the characteristics of the detected CECs in non-urban lake sites (n = 71), these compounds were checked against established criteria for potentially toxic PMs (PM(T)s) and occurrence in the aquatic environment, respectively. For the CECs with missing SSDs (n = 15 [acute], n = 41 [chronic]), ecotoxicity data were extracted for eight taxonomic groups, and if data were sufficient (n ≥ 3), SSDs were derived. The retrieved and newly developed SSDs were then used in an environmental hazard assessment (EHA) in the investigated Swedish rivers and lakes. In the rivers, 8 CECs had RQ> 1 in at least one location, and 20 CECs posed a moderate risk (0.01 < RQ < 1). In total, 21 of the 71 detected substances had already been identified as PM(T)/vPvM substances. Our study shows the importance of studying field data at large spatial scale to reveal potential environmental hazards far from source areas., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 The Authors. Published by Elsevier B.V. All rights reserved.)

To better predict the timely variation of algal blooms and other vital factors for safer drinking water production, a new AI scanning-focusing process was investigated for improving the simulation and prediction of algae counts. With a feedforward neural network (FNN) as a base, nerve cell numbers in the hidden layer and the permutation and combination of factors, etc., were fully scanned to select the best models and highly correlated factors. All the factors involved in the modeling and selection included the date (year/month/day), sensor data (temperature, pH, conductivity, turbidity, UV254-dissolved organic matter, etc.), lab measurements (algae concentration) and calculated CO 2 concentration. The new AI scanning-focusing process resulted in the best models with the most suitable key factors, which are named closed systems. In this case study, models with highest prediction performance are the (1) date-algae-temperature-pH (DATH) and (2) date-algae-temperature-CO 2 (DATC) systems. After the model selection process, the best models from both DATH and DATC were used to compare the other two methods in the modeling simulation process: the simple traditional neural network method (SP), where only date and target factor as inputs, and a blind AI training process (BP), which considers all available factors as inputs. Validation results show that all methods except BP had comparable results for algae prediction and other water quality factors, such as temperature, pH and CO 2 , among which DATC displayed an obviously poorer performance through curve fitting with original CO 2 data compared to that of SP. Therefore, DATH and SP were selected for the application test, where DATH outperformed SP due to the uncompromised performance after a long training period. Our AI scanning-focusing process and model selection showed the potential for improving water quality prediction by identifying the most suitable factors. This provides a new method to be considered in the enhancing of numerical prediction for the factors in water quality prediction and broader environment-related areas.

A wide range of organic micropollutants (n = 163) representing several compound categories (pharmaceuticals, pesticides, per- and polyfluorinated alkyl substances, flame retardants, phthalates, food additives, drugs and benzos) were analysed in water samples from the Göta Älv river (Sweden's second largest source water). The sampling also included raw water and finished drinking water from seven drinking water treatment plants and in addition a more detailed sampling at one of the treatment plants after six granulated active carbon filters of varying operational ages. In total, 27 organic micropollutants were detected, with individual concentrations ranging from sub ng L -1 levels to 54 ng L -1 . The impact of human activities along the flow path was reflected by increased concentrations downstream the river, with total concentrations ranging from 65 ng L -1 at the start of the river to 120 ng L -1 at the last sampling point. The removal efficiency was significantly (p = 0.014; one-sided t-test) higher in treatment plants that employed granulated active carbon filters (n = 4; average 60%) or artificial infiltration (n = 1; 65%) compared with those that used a more conventional treatment strategy (n = 2; 38%). The removal was also strongly affected by the operational age of the carbon filters. A filter with an operational age of 12 months with recent addition of ~10% new material showed an average removal efficiency of 92%, while a 25-month old filter had an average of 76%, and an even lower 34% was observed for a 71-month old filter. The breakthrough in the carbon filters occurred in the order of dissolved organic carbon, per- and polyfluorinated alkyl substances and then other organic micropollutants. The addition of fresh granulated active carbon seemed to improve the removal of hydrophobic organic compounds, particularly dissolved organic carbon and per- and polyfluorinated alkyl substances., (Copyright © 2019 The Authors. Published by Elsevier B.V. All rights reserved.)

Drinking water treatment plants (DWTPs) designed to remove natural organic matter (NOM) are challenged as concentrations of NOM in raw waters are increasing. Here, we assess seasonal differences in NOM quality and quantity, from raw waters to the distribution network, at three large DWTPs in Oslo, Stockholm and Helsinki. Samples, collected during stable stratification in both winter and summer and during the autumnal turnover, were analysed for NOM concentrations and composition. The NOM was characterized by common routine parameters, size and content (TFF, LC-OCD, fluorescence) and biodegradability. The NOM concentration decreased to 2.5 mg/L (55%), 4.0 mg/L (48%) and 5.7 mg/L (76%) at the respective DWTPs in Oslo, Stockholm and Helsinki. The NOM in raw waters were predominantly in the largest size fraction (>50 kDa), in particular from Oslo. High MW fractions >50 kDa and humics remained the largest fractions with minimum 30% and maximum 80% of the total NOM. The BDOC in treated water <0.3 mg/L and the conditions in the distribution network imply low probability for bacteria regrowth. The multi-step treatment consisting of coagulation/flocculation, sedimentation, rapid sand filtration, ozonation and biological activated carbon filtration (BAC) was most effective in removing NOM. Coagulation/flocculation followed by sedimentation and sand filtration were critical, especially for the removal of biopolymers and humics, and somewhat for building blocks. The sand filtration provided up to 25% additional removal of biopolymers and below 7% removal of other fractions. The ozonation and BAC was more effective and removed 11% of biopolymers, and about 35% of building blocks and LMW neutrals., (Copyright © 2019 The Authors. Published by Elsevier Ltd.. All rights reserved.)

Drinking water treatment plants (DWTPs) are constantly adapting to a host of emerging threats including the removal of micro-pollutants like perfluoroalkyl substances (PFASs), while concurrently considering how background levels of dissolved organic matter (DOM) influences their removal efficiency. Two adsorbents, namely anion exchange (AE) and granulated active carbon (GAC) have shown particular promise for PFAS removal, yet the influence of background levels of DOM remains poorly explored. Here we considered how the removal efficiency of 13 PFASs are influenced by two contrasting types of DOM at four concentrations, using both AE (Purolite A-600 ® ) and GAC (Filtrasorb 400 ® ). We placed emphasis on the pre-equilibrium conditions to gain better mechanistic insight into the dynamics between DOM, PFASs and adsorbents. We found AE to be very effective at removing both PFASs and DOM, while largely remaining resistant to even high levels of background DOM (8 mg carbon L -1 ) and surprisingly found that smaller PFASs were removed slightly more efficiently than longer chained counterparts, In contrast, PFAS removal efficiency with GAC was highly variable with PFAS chain length, often improving in the presence of DOM, but with variable response based on the type of DOM and PFAS chain length., (Copyright © 2017 Elsevier Ltd. All rights reserved.)

Symbiotic ectomycorrhizal fungi mobilize nutrients from both organic and inorganic substrates and supply them to their host plants. Their role in mobilizing base cations and phosphorus from mineral substrates through weathering has received increasing attention in recent years but the processes involved remain to be elucidated. We grew selected ectomycorrhizal and nonmycorrhizal fungi in axenic systems containing mineral and organic substrates and examined their capacity to fractionate and assimilate stable isotopes of magnesium. The mycorrhizal fungi were significantly depleted in heavy isotopes with the lowest Δ 26 Mg values (the difference between δ 26 Mg in fungal tissue and δ 26 Mg in the substrate) compared with nonmycorrhizal fungi, when grown on mineral substrates containing granite particles. The ectomycorrhizal fungi accumulated significantly higher concentrations of Mg, K and P than the nonmycorrhizal fungi. There was a highly significant statistical relationship between δ 26 Mg tissue signature and mycelial concentration of Mg, with a clear separation between most ectomycorrhizal fungi and the nonmycorrhizal fungi. These results are consistent with the idea that ectomycorrhizal fungi have evolved efficient mechanisms to mobilize, transport and store Mg within their mycelia., (© 2016 Society for Applied Microbiology and John Wiley & Sons Ltd.)

In boreal forest catchments, solute transfer to streams is controlled by hydrological and biogeochemical processes occurring in the riparian zone (RZ). However, RZs are spatially heterogeneous and information about solute chemistry is typically limited. This is problematic when making inferences about stream chemistry. Hypothetically, the strength of links between riparian and stream chemistry is time-scale dependent. Using a ten-year (2003-2012) dataset from a northern Swedish catchment, we evaluated the suitability of RZ data to infer stream dynamics at different time scales. We focus on the role of the RZ versus upslope soils in controlling sulfate (SO4(2)(-)) and dissolved organic carbon (DOC). A priori, declines in acid deposition and redox-mediated SO4(2)(-) pulses control sulfur (S) fluxes and pool dynamics, which in turn affect dissolved organic carbon (DOC). We found that the catchment is currently a net source of S, presumably due to release of the S pool accumulated during the acidification period. In both, RZ and stream, SO4(2-) concentrations are declining over time, whereas DOC is increasing. No temporal trends in SO4(2-) and DOC were observed in upslope mineral soils. SO4(2-) explained the variation of DOC in stream and RZ, but not in upslope mineral soil. Moreover, as SO4(2-) decreased with time, temporal variability of DOC increased. These observations indicate that: (1) SO4(2-) is still an important driver of DOC trends in boreal catchments and (2) RZ processes control stream SO4(2-) and subsequently DOC independently of upslope soils. These phenomena are likely occurring in many regions recovering from acidification. Because water flows through a heterogeneous mosaic of RZs before entering the stream, upscaling information from limited RZ data to the catchment level is problematic at short-time scales. However, for long-term trends and annual dynamics, the same data can provide reasonable representations of riparian processes and support meaningful inferences about stream chemistry., (Copyright © 2016 The Authors. Published by Elsevier B.V. All rights reserved.)

Rising organic matter concentrations in surface waters in many Nordic countries require current drinking water treatment processes to be adapted. Accordingly, the use of a novel nanofiltration (NF) membrane was studied during a nine month period in pilot scale at a large drinking water treatment plant in Stockholm, Sweden. A chemically resistant hollow-fibre NF membrane was fed with full scale process water from a rapid sand filter after aluminum sulfate coagulation. The combined coagulation and NF process removed more than 90% of the incoming lake water dissolved organic carbon (DOC) (8.7 mg C L(-1)), and 96% of the absorbance at 254 nm (A254) (0.28 cm(-1) incoming absorbance). Including granulated active carbon GAC) filter, the complete pilot plant treatment process we observed decreases in DOC concentration (8.7-0.5 mg C L(-1)), SUVA (3.1-1.7 mg(-1) L m(-1)), and the average nominal molecular mass (670-440 Da). Meanwhile, water hardness was practically unaffected (<20% reduction). Humic substances (HS) and biopolymers were almost completely eliminated (6510-140 and 260 to 10 μg C L(-1) respectively) and low molecular weight (LMW) neutrals decreased substantially (880-190 μg C L(-1)). Differential excitation emission matrices (EEMs), which illustrate the removal of fluorescing organic matter (FDOM) over a range of excitation and emission wavelengths, demonstrate that coagulation removed 35 ± 2% of protein-like material and 65 ± 2% of longer emission wavelength, humic-like FDOM. The subsequent NF treatment was somewhat less selective but still preferentially targeted humic-like FDOM (83 ± 1%) to a larger extent than protein-like material (66 ± 3%). The high selectivity of organic matter during coagulation compared to NF separation was confirmed from analyses with Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS), and liquid chromatography with organic carbon detection (LC-OCD), as coagulation exclusively targeted oxidized organic matter components while NF removed both chemically reduced and oxidized components. DOC removal and change in DOC character in the GAC filters showed marked differences with slower saturation and more pronounced shifts in DOC character using NF as pre-treatment. Fluorescence derived parameters showed a similar decrease over time of GAC performance for the first 150 days but also indicated ongoing change of DOM character in the post NF GAC filtrate over time even after LC-OCD indicated steady state with respect to outgoing carbon. During our trial iron concentrations were low (<30 ppb) and thus A254 could be directly related to the concentration of HS (R(2) = 0.9). The fluorescence derived freshness index (β:α) proved to be an excellent variable for estimating the fraction of HS present in all samples. Given the recommended limit of 4 mg L(-1) for chemical oxygen demand (COD) for Swedish drinking water, coagulation will need to be supplemented with one or more treatment steps irrespective whether climate change will lead to drier or wetter conditions in order to maintain sufficient DOC removal with the current increasing concentrations in raw waters., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

Absorbance, 3D fluorescence and ultrahigh resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry (ESI-FT-ICR-MS) were used to explain patterns in the removal of chromophoric and fluorescent dissolved organic matter (CDOM and FDOM) at the molecular level during drinking water production at four large drinking water treatment plants in Sweden. When dissolved organic carbon (DOC) removal was low, shifts in the dissolved organic matter (DOM) composition could not be detected with commonly used DOC-normalized parameters (e.g. specific UV254 absorbance - SUVA), but was clearly observed by using differential absorbance and fluorescence or ESI-FT-ICR-MS. In addition, we took a novel approach by identifying how optical parameters were correlated to the elemental composition of DOM by using rank correlation to connect optical properties to chemical formulas assigned to mass peaks from FT-ICR-MS analyses. Coagulation treatment selectively removed FDOM at longer emission wavelengths (450-600 nm), which significantly correlated with chemical formulas containing oxidized carbon (average carbon oxidation state ≥ 0), low hydrogen to carbon ratios (H/C: average ± SD = 0.83 ± 0.13), and abundant oxygen-containing functional groups (O/C = 0.62 ± 0.10). Slow sand filtration was less efficient in removing DOM, yet selectively targeted FDOM at shorter emission wavelengths (between 300 and 450 nm), which commonly represents algal rather than terrestrial sources. This shorter wavelength FDOM correlated with chemical formulas containing reduced carbon (average carbon oxidation state ≤ 0), with relatively few carbon-carbon double bonds (H/C = 1.32 ± 0.16) and less oxygen per carbon (O/C = 0.43 ± 0.10) than those removed during coagulation. By coupling optical approaches with FT-ICR-MS to characterize DOM, we were for the first time able to confirm the molecular composition of absorbing and fluorescing DOM selectively targeted during drinking water treatment., (Copyright © 2015 The Authors. Published by Elsevier Ltd.. All rights reserved.)

Boreal regions store most of the global terrestrial carbon, which can be transferred as dissolved organic carbon (DOC) to inland waters with implications for both aquatic ecology and carbon budgets. Headwater riparian zones (RZ) are important sources of DOC, and often just a narrow 'dominant source layer' (DSL) within the riparian profile is responsible for most of the DOC export. Two important questions arise: how long boreal RZ could sustain lateral DOC fluxes as the sole source of exported carbon and how its hydromorphological variability influences this role. We estimate theoretical turnover times by comparing carbon pools and lateral exports in the DSL of 13 riparian profiles distributed over a 69 km(2) catchment in northern Sweden. The thickness of the DSL was 36 ± 18 (average ± SD) cm. Thus, only about one-third of the 1-m-deep riparian profile contributed 90% of the lateral DOC flux. The 13 RZ exported 8.7 ± 6.5 g C m(-2) year(-1) , covering the whole range of boreal stream DOC exports. The variation could be explained by local hydromorphological characteristics including RZ width (R(2) = 0.90). The estimated theoretical turnover times were hundreds to a few thousands of years, that is there is a potential long-lasting supply of DOC. Estimates of net ecosystem production in the RZ suggest that lateral fluxes, including both organic and inorganic C, could be maintained without drawing down the riparian pools. This was supported by measurements of stream DO(14) C that indicated modern carbon as the predominant fraction exported, including streams disturbed by ditching. The transfer of DOC into boreal inland waters from new and old carbon sources has a major influence on surface water quality and global carbon balances. This study highlights the importance of local variations in RZ hydromorphology and DSL extent for future DOC fluxes under a changing climate., (© 2015 The Authors. Global Change Biology Published by John Wiley & Sons Ltd.)

Forest biofuel is a main provider of energy in Sweden and the market is expected to grow even further in the future. Removal of logging residues via harvest can lead to short-term acidification but the long-term effects are largely unknown. The objectives of this study were to 1) model the long-term effect of whole-tree harvest (WTH) on soil and stream water acidity and 2) perform sensitivity analyses by varying the amounts of logging residues, calcium (Ca(2+)) concentrations in tree biomass and site productivity in nine alternate scenarios. Data from three Swedish forested catchments and the Model of Acidification of Groundwater in Catchments (MAGIC) were used to simulate changes in forest soil exchangeable Ca(2+) pools and stream water acid neutralizing capacity (ANC) at Gammtratten, Kindla and Aneboda. Large depletions in soil Ca(2+) supply and a reversal of the positive trend in stream ANC were predicted for all three sites after WTH. However, the magnitude of impact on stream ANC varied depending on site and the concentration of mobile strong acid anions. Contrary to common beliefs, the largest decrease in modelled ANC was observed at the well-buffered site Gammtratten. The effects at Kindla and Aneboda were much more limited and not large enough to offset the general recovery from acidification. Varying the tree biomass Ca(2+) concentrations exerted the largest impact on modelled outcome. Site productivity was the second most important variable whereas changing biomass amounts left on site only marginally affected the results. The outcome from the sensitivity analyses pointed in the same direction of change as in the base scenario, except for Kindla where soil Ca(2+) pools were predicted to be replenished under a given set of input data. The reliability of modelled outcome would increase by using site-specific Ca(2+) concentrations in tree biomass and field determined identification of site productivity., (Copyright © 2014 Elsevier B.V. All rights reserved.)

Quantifying the effects of human activity on the natural environment is dependent on credible estimates of reference conditions to define the state of the environment before the onset of adverse human impacts. In Europe, emission controls that aimed at restoring ecological status were based on hindcasts from process-based models or paleolimnological reconstructions. For instance, 1860 is used in Europe as the target for restoration from acidification concerning biological and chemical parameters. A more practical problem is that the historical states of ecosystems and their function cannot be observed directly. Therefore, we (i) compare estimates of acidification based on long-term observations of roach (Rutilus rutilus) populations with hindcast pH from the hydrogeochemical model MAGIC; (ii) discuss policy implications and possible scope for use of long-term archival data for assessing human impacts on the natural environment and (iii) present a novel conceptual model for interpreting the importance of physico-chemical and ecological deviations from reference conditions. Of the 85 lakes studied, 78 were coherently classified by both methods. In 1980, 28 lakes were classified as acidified with the MAGIC model, however, roach was present in 14 of these. In 2010, MAGIC predicted chemical recovery in 50% of the lakes, however roach only recolonized in five lakes after 1990, showing a lag between chemical and biological recovery. Our study is the first study of its kind to use long-term archival biological data in concert with hydrogeochemical modeling for regional assessments of anthropogenic acidification. Based on our results, we show how the conceptual model can be used to understand and prioritize management of physico-chemical and ecological effects of anthropogenic stressors on surface water quality., (© 2014 The Authors Global Change Biology Published by John Wiley & Sons Ltd.)

Inland waters transport large amounts of dissolved organic matter (DOM) from terrestrial environments to the oceans, but DOM also reacts en route, with substantial water column losses by mineralization and sedimentation. For DOM transformations along the aquatic continuum, lakes play an important role as they retain waters in the landscape allowing for more time to alter DOM. We know DOM losses are significant at the global scale, yet little is known about how the reactivity of DOM varies across landscapes and climates. DOM reactivity is inherently linked to its chemical composition. We used fluorescence spectroscopy to explore DOM quality from 560 lakes distributed across Sweden and encompassed a wide climatic gradient typical of the boreal ecozone. Six fluorescence components were identified using parallel factor analysis (PARAFAC). The intensity and relative abundance of these components were analyzed in relation to lake chemistry, catchment, and climate characteristics. Land cover, particularly the percentage of water in the catchment, was a primary factor explaining variability in PARAFAC components. Likewise, lake water retention time influenced DOM quality. These results suggest that processes occurring in upstream water bodies, in addition to the lake itself, have a dominant influence on DOM quality. PARAFAC components with longer emission wavelengths, or red-shifted components, were most reactive. In contrast, protein-like components were most persistent within lakes. Generalized characteristics of PARAFAC components based on emission wavelength could ease future interpretation of fluorescence spectra. An important secondary influence on DOM quality was mean annual temperature, which ranged between -6.2 and +7.5 °C. These results suggest that DOM reactivity depends more heavily on the duration of time taken to pass through the landscape, rather than temperature. Projected increases in runoff in the boreal region may force lake DOM toward a higher overall amount and proportion of humic-like substances., (© 2013 The Authors Global Change Biology Published by John Wiley & Sons Ltd.)

Stream water concentrations of 13 major and trace elements (Al, Ba, Ca, Cr, Cu, La, Mg, Na, Ni, Si, Sr, U, Y) were used to estimate fluxes from 15 boreal catchments. All elements displayed a significant negative correlation to the wetland coverage, but the influence of wetlands was stronger for organophilic metals; 73% of the spatial differences in the normalized element fluxes could be explained based only on the wetland coverage and the affinity for organic matter, which was quantified using thermodynamic modeling. When the analysis was restrained to the smaller streams (<10 km(2)) the explanatory power increased to 88%. The results suggest that wetlands may decrease the fluxes of metals from boreal forests to downstream recipients by up to 40% at otherwise similar runoff. We suggest that the decrease in element fluxes is caused by a combination of low weathering in peat soils and accumulation of organophilic metals in peat. The model could not explain the spatial patterns for some metals with low affinity for organic matter, some redox-sensitive metals, and some metals with exceptionally high atmospheric deposition, but the results still demonstrate that wetlands play an important role for the biogeochemical cycling of many metals in the boreal landscape.

The recent browning (increase in color) of surface waters across much of the northern hemisphere has important implications for light climate, ecosystem functioning, and drinking water treatability. Using log-linear regressions and long-term (6-21 years) data from 112 Swedish watercourses, we identified temporal and spatial patterns in browning-related parameters [iron, absorbance, and total organic carbon (TOC)]. Flow variability and lakes in the catchment were major influences on all parameters. Co-variation between seasonal, discharge-related, and trend effects on iron, TOC, and absorbance were dependent on pH, landscape position, catchment size, latitude, and dominant land cover. Large agriculture-dominated catchments had significantly larger trends in iron, TOC, and water color than small forest catchments. Our results suggest that while similarities exist, no single mechanism can explain the observed browning but show that multiple mechanisms related to land cover, climate, and acidification history are responsible for the ongoing browning of surface waters.

Long-term (1987-2012) water quality monitoring in 36 acid-sensitive Swedish lakes shows slow recovery from historic acidification. Overall, strong acid anion concentrations declined, primarily as a result of declines in sulfate. Chloride is now the dominant anion in many acid-sensitive lakes. Base cation concentrations have declined less rapidly than strong acid anion concentrations, leading to an increase in charge balance acid neutralizing capacity. In many lakes, modeled organic acidity is now approximately equal to inorganic acidity. The observed trends in water chemistry suggest lakes may not return to reference conditions. Despite declines in acid deposition, many of these lakes are still acidified. Base cation concentrations continue to decline and alkalinity shows only small increases. A changing climate may further delay recovery by increasing dissolved organic carbon concentrations and sea-salt episodes. More intensive forest harvesting may also hamper recovery by reducing the supply of soil base cations.

Increased color in surface waters, or browning, can alter lake ecological function, lake thermal stratification and pose difficulties for drinking water treatment. Mechanisms suggested to cause browning include increased dissolved organic carbon (DOC) and iron concentrations, as well as a shift to more colored DOC. While browning of surface waters is widespread and well documented, little is known about why some lakes resist it. Here, we present a comprehensive study of Mälaren, the third largest lake in Sweden. In Mälaren, the vast majority of water and DOC enters a western lake basin, and after approximately 2.8 years, drains from an eastern basin. Despite 40 years of increased terrestrial inputs of colored substances to western lake basins, the eastern basin has resisted browning over this time period. Here we find the half-life of iron was far shorter (0.6 years) than colored organic matter (A₄₂₀; 1.7 years) and DOC as a whole (6.1 years). We found changes in filtered iron concentrations relate strongly to the observed loss of color in the western basins. In addition, we observed a substantial shift from colored DOC of terrestrial origin, to less colored autochthonous sources, with a substantial decrease in aromaticity (-17%) across the lake. We suggest that rapid losses of iron and colored DOC caused the limited browning observed in eastern lake basins. Across a wider dataset of 69 Swedish lakes, we observed greatest browning in acidic lakes with shorter retention times (< 1.5 years). These findings suggest that water residence time, along with iron, pH and colored DOC may be of central importance when modeling and projecting changes in brownification on broader spatial scales.

Riverine transport of iron (Fe) and arsenic (As) is affected by their associations with natural organic matter (NOM) and suspended iron (oxy)hydroxides. Speciation has a strong influence on element transport from the headwaters to the ocean because NOM may be transported over longer distances compared to iron (oxy)hydroxides. We show that Fe speciation changes along the flow path of a boreal watercourse, as water moves from NOM-rich, acidic first-order streams with pH as low as 3.9 to less acidic higher-order systems (up to pH 6.4). Analysis by Flow Field-Flow Fractionation and chemical equilibrium modeling revealed that Fe from wetland-dominated headwaters was mainly exported as Fe-NOM complexes; in catchments with a stream order >1 and with higher pH, Fe was present in Fe-NOM complexes and precipitated as nanoparticulate iron(oxy)hydroxides which aggregated as the pH increased, with their size eventually exceeding the membrane filters cutoff (0.2 μm). The measured NOM-bound Fe decreased with increasing pH, from 0.38 to 0.16 mmol Fe·g(NOM)(-1). The high concentrations of NOM-bound Fe emphasize the importance of boreal catchments to Fe export to the oceans. Concentrations of As in the <0.2 μm fraction but larger than what is usually considered "truly dissolved" (<1000 g·mol(-1)), decreased from 75% to 26% with increasing pH. The As in this size range was mainly associated with NOM but at pH >4.5 became associated with iron(oxy)hydroxides, and its transport thus became more coupled to that of the iron(oxy)hydroxides downstream in the circumneutral streams.

Natural organic matter (NOM) serve as precursors for disinfection byproducts (DBPs) in drinking water production making NOM removal essential in predisinfection treatment processes. We identified molecular formulas of chlorinated DBPs after chlorination and chloramination in four Swedish surface water treatment plants (WTPs) using ultrahigh resolution Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS). Chlorine-containing formulas were detected before and after disinfection and were therefore classified to identify DBPs. In total, 499 DBPs were detected, of which 230 have not been reported earlier. The byproducts had, as a group, significantly lower ratio of hydrogen to carbon (H/C) and significantly higher average carbon oxidation state (COS), double bond equivalents per carbon (DBE/C) and ratio of oxygen to carbon (O/C) compared to Cl-containing components present before disinfection and CHO formulas in samples taken both before and after disinfection. Electrophilic substitution, the proposed most significant reaction pathway for chlorination of NOM, results in carbon oxidation and decreased H/C while O/C and DBE/C is left unchanged. Because the identified DBPs had significantly higher DBE/C and O/C than the CHO formulas we concluded that chlorination of NOM during disinfection is selective toward components with relatively high double bond equivalency and number of oxygen atoms per carbon. Furthermore, choice of disinfectant, dose, and predisinfection treatment at the different WTPs resulted in distinct patterns in the occurrence of DBP formulas.

Ultraviolet/visible (UV/Vis) absorbance spectroscopy is a commonly used technique for characterizing dissolved organic matter (DOM). We present an analysis of UV/Vis absorbance spectra from 983 lakes throughout Sweden, sampled during autumn 2009. Metrics included both specific absorbances (i.e. absorbance per mass unit of organic carbon), and descriptions of spectral shape. Overall, we found three factors to which all spectral metrics were similarly related: acidity, retention-time, and latitude. In general, alkaline lakes with a long retention time in northern Sweden have lower specific absorbance and steeper spectral slope than acidic lakes with a short retention time in southern Sweden. Relative to the specific absorbance measured at 254 nm (SUVA), commonly used as a measure of DOM aromaticity, the specific absorbance at longer wavelengths and metrics of spectral shape were more sensitive to acidity and less sensitive to latitude. Although different spectral metrics are hypothesized to reflect different properties of DOM, UV/Vis absorbance spectroscopy may not be useful for more refined characterization of organic matter because of the strong inter-correlation between metrics. Nevertheless, it remains useful as a quick, cheap and reliable method of estimating DOM quantity and describing quality. We suggest that the most informative range to measure absorbance is between approximately 250 and 360 nm, where the between-lake variability is largest and absorbance can, in general, be precisely measured.

Surface waters are the main source of drinking water in many regions. Increasing organic carbon concentrations are a cause for concern in Nordic countries since both dissolved and particulate organic carbon can transport contaminants and adversely affect drinking water treatment processes. We present a long-term study of dynamics of total (particulate and dissolved) organic carbon (TOC) concentrations in the River Fyris. This river supplies drinking water to approximately 200000 people in Uppsala, Sweden. The River Fyris is a main tributary to Lake Mälaren, which supplies drinking water to approximately 2 million people in the greater Stockholm area. Utilities responsible for drinking water supply in both Uppsala and Stockholm have expressed concerns about possible increases in TOC. We evaluate organic carbon dynamics within the Fyris catchment by calculating areal mass exports using observed TOC concentrations and modeled flows and by modeling dissolved organic carbon (as a proxy for TOC) using the dynamic, process based INCA-C model. Exports of TOC from the catchment ranged from 0.8 to 5.8 g m(-2) year(-1) in the period 1995-2010. The variation in annual exports was related to climatic variability which influenced seasonality and amount of runoff. Exports and discharge uncoupled at the end of 2008. A dramatic increase in TOC concentrations was observed in 2009, which gradually declined in 2010-2011. INCA-C successfully reproduced the intra- and inter-annual variation in concentrations during 1996-2008 and 2010-2011 but failed to capture the anomalous increase in 2009. We evaluated a number of hypotheses to explain the anomaly in 2009 TOC values, ultimately none proved satisfactory. We draw two main conclusions: there is at least one unknown or unmeasured process controlling or influencing surface water TOC and INCA-C can be used as part of the decision-making process for current and future use of rivers for drinking water supply., (Copyright © 2012 Elsevier B.V. All rights reserved.)

In order to apply Sr/Ca and (44)Ca/(40)Ca fractionation during calcium carbonate (CaCO(3)) formation as a proxy to reconstruct paleo-environments, it is essential to evaluate the impact of various environmental factors. In this study, a CO(2) diffusion technique was used to crystallize inorganic calcite from aqueous solutions at different ionic strength/salinity by the addition of NaCl at 25 °C. Results show that the discrimination of Sr(2+) versus Ca(2+) during calcite formation is mainly controlled by precipitation rate (R in μmol/m(2)/h) and is weakly influenced by ionic strength/salinity. In analogy to Sr incorporation, (44)Ca/(40)Ca fractionation during precipitation of calcite is weakly influenced by ionic strength/salinity too. At 25 °C the calcium isotope fractionation between calcite and aqueous calcium ions (Δ(44/40)Ca(calcite-aq) = δ(44/40)Ca(calcite) - δ(44/40)Ca(aq)) correlates inversely to log R values for all experiments. In addition, an inverse relationship between Δ(44/40)Ca(calcite-aq) and log D(Sr), which is independent of temperature, precipitation rate, and aqueous (Sr/Ca)(aq) ratio, is not affected by ionic strength/salinity either. Considering the log D(Sr) and Δ(44/40)Ca(calcite-aq) relationship, Sr/Ca and δ(44/40)Ca(calcite) values of precipitated calcite can be used as an excellent multi-proxy approach to reconstruct environmental conditions (e.g., temperature, precipitation rate) of calcite growth and diagenetic alteration.

Long-term (1860-2010) catchment mass balance calculations rely on models and assumptions which are sources of uncertainty in acidification assessments. In this article, we report on an application of MAGIC to model acidification at the four Swedish IM forested catchments that have been subject to differing degrees of acidification stress. Uncertainties in the modeled mass balances were mainly associated with the deposition scenario and assumptions about sulfate adsorption and soil mass. Estimated base cation (BC) release rates (weathering) varied in a relatively narrow range of 47-62 or 42-47 meq m(-2) year(-1), depending on assumptions made about soil cation exchange capacity and base saturation. By varying aluminum solubility or introducing a dynamic weathering feedback that allowed BC release to increase at more acidic pHs, a systematic effect on predicted changes in acid neutralizing capacity (ΔANC ca. 10-41 μeq l(-1)) and pH (ca. ΔpH = 0.1-0.6) at all sites was observed. More robust projections of future changes in pH and ANC are dependent on reducing uncertainties in BC release rates, the timing, and extent of natural acidification through BC uptake by plants, temporal changes in soil element pools, and fluxes of Al between compartments.

Surface water concentrations of dissolved organic carbon ([DOC]) are changing throughout the northern hemisphere due to changes in climate, land use and acid deposition. However, the relative importance of these drivers is unclear. Here, we use the Integrated Catchments model for Carbon (INCA-C) to simulate long-term (1996-2008) streamwater [DOC] at the four Swedish integrated monitoring (IM) sites. These are unmanaged headwater catchments with old-growth forests and no major changes in land use. Daily, seasonal and long-term variations in streamwater [DOC] driven by runoff, seasonal temperature and atmospheric sulfate (SO₄(2-)) deposition were observed at all sites. Using INCA-C, it was possible to reproduce observed patterns of variability in streamwater [DOC] at the four IM sites. Runoff was found to be the main short-term control on [DOC]. Seasonal patterns in [DOC] were controlled primarily by soil temperature. Measured SO₄(2-) deposition explained some of the long-term [DOC] variability at all sites.

A consistent chemical equilibrium model that calculates pH from charge balance constraints and aluminum and iron speciation in the presence of natural organic matter is presented. The model requires input data for total aluminum, iron, organic carbon, fluoride, sulfate, and charge balance ANC. The model is calibrated to pH measurements (n = 322) by adjusting the fraction of active organic matter only, which results in an error of pH prediction on average below 0.2 pH units. The small systematic discrepancy between the analytical results for the monomeric aluminum fractionation and the model results is corrected for separately for two different fractionation techniques (n = 499) and validated on a large number (n = 3419) of geographically widely spread samples all over Sweden. The resulting average error for inorganic monomeric aluminum is around 1 µM. In its present form the model is the first internally consistent modeling approach for Sweden and may now be used as a tool for environmental quality management. Soil gibbsite with a log *Ks of 8.29 at 25°C together with a pH dependent loading function that uses molar Al/C ratios describes the amount of aluminum in solution in the presence of organic matter if the pH is roughly above 6.0.

The effect of dissolved Zn, Co, Pb, Mg, and Ca on the uptake of cadmium by biogenic aragonite was investigated. Experiments were performed in batch-reactors using metal-cadmium-bearing solutions and shell fragments with diameters in different ranges, the solid/liquid ratio being 10 grams per liter. Different initial concentrations of cadmium and metals (1.0-0.005 mM) were used. Uptake takes place via heterogeneous nucleation of metal-bearing crystallites onto the shell surfaces. Cadmium removal occurs by surface precipitation of otavite. Under the conditions used here, Co and Ca as well as Pb < or = 0.3 mM and Zn < or = 0.3 mM do not have a significant effect on the removal of cadmium. At higher concentrations, Pb and Zn outcompete Cd for the dissolving carbonate ions and thus decrease significantly the Cd removal rates. In contrast, Mg has a slight enhancing effect. Pb and Zn are removed faster than Cd, precipitating as PbCO3, Pb3(CO3)2(OH)2, and Zn5(CO3)2(OH)6. Within 24-72 h, the concentrations of lead, cadmium, and zinc decrease until approximately 0.5 microM, and the presence of aragonite buffers the solution to a pH above 8 avoiding redissolution. The study demonstrates the high effectiveness of biogenic aragonite in removing Cd and other metals from polluted waters.