Carbon budgets for catchments across a managed landscape mosaic in southeast Sweden: contributing to the safety assessment of a nuclear waste repository

Ecosystem budgets of matter contribute to the assessment of transport and accumulation of bioavailable contaminants in a landscape, since flows of matter and energy ultimately determine the rates at which contaminants will be partitioned in the environment. This study compares ecosystem properties, such as net primary production (NPP), sequestration of matter and fluxes to food sources for humans, which are of potential interest to describe fluxes and accumulation of bioavailable radionuclides in 14 catchments within a larger catchment area in southeast Sweden. The carbon budgets, used as a proxy for organic matter, are mainly based on local estimates of pools and fluxes, which have been distributed across a landscape mosaic of different vegetation types and management regimes using a geographical information system (GIS). NPP varied by a factor close to two (432 - 709 g x Cx m(-2)x y(-1)), while net ecosystem production ranged between -124 and 159 gx C x m(-2) x y (-1) for the different catchments. Carbon sequestration mainly occurred in the vegetation while the soil organic carbon pool was mainly a source of carbon. Large herbivores consumed on average 4.5 % of the above-ground green tissue production. When arable land was present in the catchment, the flux of carbon to humans was highest from crops and, in decreasing order, milk and beef, followed by the flux from hunting and berry/fungus picking. The results can be used to estimate the potential assimilation of radionuclides in vegetation and the potential exposure to humans of bioavailable radionuclides.     

The use of a high-FeO olivine rock as a redox buffer in a nuclear waste repository

Due to the higher stability of the spent nuclear fuel (mainly composed of UO2) under reducing conditions, and in order to enhance the retention/retardation of some key radionuclides, the olivine rock from the Lovasj?rvi intrusion has been proposed as a potential redox-active backfill-additive in deep high-level nuclear waste (HLNW) repositories. In this work, two different approaches have been undertaken in order to establish the redox buffer capacity of olivine rock: (1) The capacity of the rock to respond to changes in pH or pe has been demonstrated and the final (pH, pe) coordinates agree with the control exerted by the system Fe(II)/Fe(III). (2) The rate of consumption of oxygen has been determined at different pH values. These rates are higher than the ones reported in the literature for other solids, what would point to the possibility of using this rock as an additive to the backfill material in a HLNW.     

Description, assessment and meaning of vertical fluxes of matter within ecotopes: a systematic consideration

Ecotopes are the structural elements of landscapes for which matter and energy balances can be derived from measurements. Vertical flux densities are the typical entities governing their structure and function. Potential flux densities in ecotopes are discussed in detail using a complex circuit diagram that differentiates between transport and reaction columnar resistors. From this the locations and methods of measurement are deduced. Determination of flux densities between troposphere and phytosphere/pedosphere is restricted to the constant flux layer, by theory and practice.     

A carbon budget of a small humic lake: an example of the importance of lakes for organic matter cycling in boreal catchments

Lakes play an important role in the cycling of organic matter in the boreal landscape, due to the frequently high extent of bacterial respiration and the efficient burial of organic carbon in sediments. Based on a mass balance approach, we calculated a carbon budget for a small humic Swedish lake in the vicinity of a potential final repository for radioactive waste in Sweden, in order to assess its potential impact on the environmental fate of radionuclides associated with organic matter. We found that the lake is a net heterotrophic ecosystem, subsidized by organic carbon inputs from the catchment and from emergent macrophyte production. The largest sink of organic carbon is respiration by aquatic bacteria and subsequent emission of carbon.dioxide to the atmosphere. Although the annual burial of organic carbon in the sediment is a comparatively small sink, it results in the build-up of the largest carbon pool in the lake. Hence, lakes may simultaneously disperse and accumulate organic-associated radionuclides leaking from a final repository.     

Absorption and fluorescence properties of chromophoric dissolved organic matter: implications for the monitoring of water quality in a large subtropical reservoir

The development of techniques for real-time monitoring of water quality is of great importance for effectively managing inland water resources. In this study, we first analyzed the absorption and fluorescence properties in a large subtropical reservoir and then used a chromophoric dissolved organic matter (CDOM) fluorescence monitoring sensor to predict several water quality parameters including the total nitrogen (TN), total phosphorus (TP), chemical oxygen demand (COD), dissolved organic carbon (DOC), and CDOM fluorescence parallel factor analysis (PARAFAC) components in the reservoir. The CDOM absorption coefficient at 254 nm (a(254)), the humic-like component (C1), and the tryptophan-like component (C3) decreased significantly along a gradient from the northwest to the lake center, northeast, southwest, and southeast region in the reservoir. However, no significant spatial difference was found for the tyrosine-like component (C2), which contributed only four marked peaks. A highly significant linear correlation was found between the a(254) and CDOM concentration measured using the CDOM fluorescence sensor (r ²?=?0.865, n?=?76, p?相似文献   

Modeling the photo-oxidation of dissolved organic matter by ultraviolet radiation in freshwater lakes: implications for mercury bioavailability

Uncertainties in projected ultraviolet (UV) radiation may lead to future increases in UV irradiation of freshwater lakes. Because dissolved organic carbon (DOC) is the main binding phase for mercury (Hg) in freshwater lakes, an increase in DOC photo-oxidation may affect Hg speciation and bioavailability. We quantified the effect of DOC concentration on the rate of abiotic DOC photo-oxidation for five lakes (DOC=3.27-12.3 mg L(-1)) in Kejimkujik National Park, Canada. Samples were irradiated with UV-A or UV-B radiation over a 72-h period. UV-B radiation was found to be 2.36 times more efficient at photo-oxidizing DOC than UV-A, with energy-normalized rates of dissolved inorganic carbon (DIC) production ranging from 3.8×10(-5) to 1.1×10(-4) mg L(-1)J(-1) for UV-A, and from 6.0×10(-5) to 3.1×10(-4) mg L(-1)J(-1) for UV-B. Energy normalized rates of DIC production were positively correlated with DOC concentrations. Diffuse integrated attenuation coefficients were quantified in situ (UV-A K(d)=0.056-0.180 J cm(-1); UV-B K(d)=0.015-0.165 J cm(-1)) and a quantitative depth-integrated model for yearly DIC photo-production in each lake was developed. The model predicts that, UV-A produces between 3.2 and 100 times more DIC (1521-2851 mg m(-2) year(-1)) than UV-B radiation (29.17-746.7 mg m(-2) year(-1)). Future increases in UV radiation may increase DIC production and increase Hg bioavailability in low DOC lakes to a greater extent than in high DOC lakes.     

Mobilization of soil organic matter by complexing agents and implications for polycyclic aromatic hydrocarbon desorption

Complexing agents are frequently used in treatment technologies to remediate soils, sediments and wastes contaminated with toxic metals. The present study reports results that indicate that the rate and extent of soil organic matter (SOM) as represented by dissolved natural organic carbon (DNOC) and polycyclic aromatic hydrocarbon (PAH) desorption from a contaminated soil from a manufactured gas plant (MGP) site can be significantly enhanced with the aid of complexing agents. Desorption of DNOC and PAH compounds was pH dependent, with minimal release occurring at pH 2-3 and maximal release at pH 7-8. At pH-6, chelate solutions were shown to dissolve large amounts of humic substances from the soil compared to controls. The complexing agents mobilized polyvalent metal ions, particularly Fe and Al from the soil. Metal ion chelation may disrupt humic (metal ion)-mineral linkages, resulting in mobilization of SOM and accompanying PAH molecules into the aqueous phase; and/or reduce the degree of cross-linking in the soil organic matter phase, which could accelerate PAH diffusion.     

Influences of adding easily degradable organic waste on the minimization and humification of organic matter during straw composting

To find a better composting process with low greenhouse gas emission and high humus production, the effect of adding kitchen waste on reduction and humification of organic matter during straw composting was studied. Three processes were compared, consisting of different ratios of straw and kitchen waste (1:2, 1:1, and 2:1). At four time points over a 62-d incubation, the reduction and humification of compost was evaluated by measuring the total mass, carbon content, and humic material content of the compost. Treatment 1 (straw/kitchen waste ratio of 1:2) reduced the total mass of compost the most. Treatment 2 (straw/kitchen waste ratio of 1:1) reduced the total carbon content the most, reflecting the highest emission of greenhouse gas. Treatment 3 produced the most humic acid material and released the lowest amount of carbon. Hence, from the point of view of reducing greenhouse gas emissions and increasing stable organic matter such as humus and humic acid during composting, treatment #3 was optimal. The three treatments resulted in significant differences in microbial biomass and enzyme activity during composting. The highest amount of active microbial biomass was associated with the largest reduction in compost mass (treatment 1). Higher proportions of straw (treatments 2 and 3), which contains more lignin, were associated with greater β-glycosidase activity, which may generate more humus that can improve soil quality. Dehydrogenase activity seemed to be the most important microbial factor in organic carbon catabolism or humification.     

Genotoxicity of organic extracts of urban airborne particulate matter: an assessment within a personal exposure study

Airborne particulate matter, PM(10) and PM(2.5), are associated with a range of health effects including lung cancer. Their complex organic fraction contains genotoxic and carcinogenic compounds such as polycyclic aromatic hydrocarbons (PAHs) and their derivatives. This study evaluates the genotoxicity of the PM(10) and PM(2.5) organic extracts that were sampled in the framework of a personal exposure study in three French metropolitan areas (Paris, Rouen and Strasbourg), using the comet assay, performed on HeLa S3 cells. In each city, 60-90 non-smoking volunteers composed of two groups of equal size (adults and children) carried the personal Harvard Chempass multi-pollutant sampler during 48h along two different seasons ('hot' and 'cold'). Volunteers were selected so as to live (home and work/school) in 3 different urban sectors contrasted in terms of air pollution within each city (one highly exposed to traffic emissions, one influenced by local industrial sources, and a background urban environment). Genotoxic effects are stronger for PM(2.5) extracts than for PM(10), and greater in winter than in summer. Fine particles collected by subjects living within the traffic proximity sector present the strongest genotoxic responses, especially in the Paris metropolitan area. This work confirms the genotoxic potency of particulate matter (PM(10) and PM(2.5)) organic extracts to which urban populations are exposed.     

Cosorption study of organic pollutants and dissolved organic matter in a soil

In this study we have evaluated the effects of dissolved organic matter (DOM) on sorption of imidacloprid, 3,4-dichloroaniline (3,4-DCA) and 4-bromoaniline (4-BA) on a typical calcareous soil (Luvic Xerosol) from south-eastern Spain. Two different types of DOM were used, that is to say, dissolved natural organic matter extracts from a commercial peat (DNOM) and a high-purity tannic acid (TA) solution. The experiments were carried out in a 0.01 M CaCl2 aqueous medium at 25 degrees C. The results indicated that the presence of both DNOM and TA, over a concentration range of 15-100 mg L(-1), produced an increase in the amount of 3,4-DCA and 4-BA sorbed and a decrease in the amount of imidacloprid retained on the soil studied. A modified distribution coefficient, K(doc), has been proposed as a safer parameter for soil sorption predictions of organic pollutants and it could be of help to model the fate of these in the environment.     

Copper complexation by dissolved organic matter and uncertainty assessment of their stability constants

The interaction of Cu with dissolved organic matter (DOM, extracted from an organic forest floor) was investigated and the resulting data was evaluated in terms of their uncertainty. The speciation of Cu over ‘free’ Cu (as analysed by diffusive gradients in thin films (DGT)), dissolved Cu–DOM complexes and precipitated Cu–DOM was determined as a function of pH (3.5, 4.0 and 4.5) and Cu/C ratio. The dissolved organically bound fraction was highest at pH 4.5, but this fraction decreased with increasing Cu/C ratio, which was observed for all pH levels. In the range of Cu/C=7×10⁻⁵–2.3×10⁻² (mol/mol) the precipitated fraction was very small. The speciation of both Al and Fe was not affected by increasing Cu concentrations. From a continuous distribution model using the Scatchard approach, we calculated the optimal fit and corresponding upper and lower 95% uncertainty bounds of the overall stability constants (K_o) with the shuffled complex evolution Metropolis (SCEM) algorithm. Although the optimal equation fitted the data very well, the uncertainty of the, according to literature, most reliable approach to establish stability constants, was still large. Accordingly, the usually reported intrinsic stability constants exhibited large uncertainty ranging from logK_i=6.0–7.1 (optimal 6.7) for pH 3.5, logK_i=6.5–7.1 (optimal 6.8) for pH 4.0, and logK_i=6.4–7.2 (optimal 6.8) for pH 4.5 and showed only little effect of pH.     

Nitrogen deposition and the biodiversity of boreal forests: implications for the nitrogen critical load

The critical load concept is used to establish the deposition levels which ecosystems can tolerate without significant harmful effects. Here we summarize work within the Swedish research program Abatement Strategies for Transboundary Air Pollution (ASTA) assessing the critical load of N for boreal forests. Results from both field experiments in an area with low background N deposition in northern Sweden, and from a large-scale monitoring study, show that important vegetational changes start to take place when adding low N doses and that recovery of the vegetation after ceasing N input is a very slow process. The data presented indicate that changes in key ecosystem components occur even at a lower rate of N input than the present recommended empirical critical load for boreal forest understorey vegetation of 10-15 kg N ha(-1) yr(-1). Based on the data presented, we suggest that the critical load should be lowered to 6 kg N ha(-1) yr(-1).     

Modelling geochemical and microbial consumption of dissolved oxygen after backfilling a high level radiactive waste repository

Dissolved oxygen (DO) left in the voids of buffer and backfill materials of a deep geological high level radioactive waste (HLW) repository could cause canister corrosion. Available data from laboratory and in situ experiments indicate that microbes play a substantial role in controlling redox conditions near a HLW repository. This paper presents the application of a coupled hydro-bio-geochemical model to evaluate geochemical and microbial consumption of DO in bentonite porewater after backfilling of a HLW repository designed according to the Swedish reference concept. In addition to geochemical reactions, the model accounts for dissolved organic carbon (DOC) respiration and methane oxidation. Parameters for microbial processes were derived from calibration of the REX in situ experiment carried out at the Asp? underground laboratory. The role of geochemical and microbial processes in consuming DO is evaluated for several scenarios. Numerical results show that both geochemical and microbial processes are relevant for DO consumption. However, the time needed to consume the DO trapped in the bentonite buffer decreases dramatically from several hundreds of years when only geochemical processes are considered to a few weeks when both geochemical reactions and microbially-mediated DOC respiration and methane oxidation are taken into account simultaneously.     

Changes in the chemical composition of water-extractable organic matter during composting: distribution between stable and labile organic matter pools

Aerobic decomposition and stabilization of organic matter during the composting of waste materials is primarily due to the biochemical transformation of water-soluble compounds in the liquid phase by the microbial biomass. For this reason water-soluble organic matter represents the most active fraction of compost, both biologically and chemically, and thus should directly reflect the biochemical alteration of organic matter. This work aims to elucidate the microbial-mediated processes responsible for the distribution of soluble organic matter between stable and labile pools with composting time. Accordingly, chemical analysis as well as UV absorption, and ¹H and ¹³C-NMR spectroscopy of samples collected during the industrial composting of urban waste revealed microbial induced transformation of water-extractable organic matter over time. The chemical composition changed from labile, hydrophilic, plant-derived organic compounds in the beginning to predominately stable, hydrophobic moieties comprising lignin-derived phenols and microbially-derived carbohydrates at later stages of composting.     

Persistent organic pollutants and sedimentary organic matter properties: a case study in the Kishon River, Israel

The Kishon River, the second largest coastal river in Israel, has been severely polluted for several decades. Sediments from upstream and downstream sites of the river were analyzed, lipid-extracted and evaluated for phenanthrene uptake. Total polycyclic aromatic hydrocarbon (PAH) concentration in downstream sediments was 299 microg kg(-1), consisting mostly of petrogenic-derived PAHs. Downstream sedimentary lipids were found to be dominated by fresh and decomposed petroleum-derived n-alkanes. The total PAH concentration in upstream sediments was 173 microg kg(-1), consisting mostly of pyrogenic-derived PAHs, whereas lipids from these sediments were mostly vegetation-derived. Spectroscopic data suggested an exceptionally high aromatic content in downstream humic acid, which originated from PAHs attached to its structure. Sorption data suggested that upstream sedimentary cuticle-derived lipids function as a sorption domain, while downstream sedimentary lipids, consisting of shorter-chain-length petroleum-derived alkanes, compete with phenanthrene for sorption sites.     

长江水体溶解有机质与金属离子作用污染分析

将万州区牌楼段的长江水与金属离子混合,通过测定荧光光谱得出,在金属离子质量浓度较低(1.0×10-7 mg/mL)时,长江水中的腐殖质与金属离子发生螯合作用而使荧光强度降低,而在更高浓度时,则由于吸附/解吸作用而使荧光强度增强.三维荧光谱图的测定结果表明,金属离子浓度的大小决定了其与腐殖质的基团反应类型.实验结果表明,...     

Impact of peri-urban landscape on the organic and mineral contamination of pond waters and related risk assessment

Environmental Science and Pollution Research - Ponds are important for their ecological value and for the ecosystem services they provide to human societies, but they are strongly affected by human...     

On the decline of ground lichen forests in the Swedish boreal landscape: Implications for reindeer husbandry and sustainable forest management

Lichens are a bottleneck resource for circumpolar populations of reindeer, and as such, for reindeer husbandry as an indigenous Sami land-use tradition in northern Sweden. This study uses ground lichen data and forest information collected within the Swedish National Forest Inventory since 1953, on the scale of northern Sweden. We found a 71 % decline in the area of lichen-abundant forests over the last 60 years. A decline was observed in all regions and age classes and especially coincided with a decrease of >60 year old, open pine forests, which was the primary explanatory factor in our model. The effects of reindeer numbers were inconclusive in explaining the decrease in lichen-abundant forest. The role that forestry has played in causing this decline can be debated, but forestry can have a significant role in reversing the trend and improving ground lichen conditions.

Electronic supplementary material

The online version of this article (doi:10.1007/s13280-015-0759-0) contains supplementary material, which is available to authorized users.