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Nitrification and denitrification are traditionally assumed to occur under aerobic and anoxic conditions, respectively. However, new and interesting alternatives challenge the traditional assumption. Along this line, we provide dual-nitrate isotopic and chemical evidence for the occurrence of denitrification linked with heterotrophic nitrification in an upper oxic region and nitrification in an underlying low-oxygen (sub-oxic/anoxic) layer of a stratified and channelized alluvial aquifer. Particularly significant is the source of the oxidant required for nitrification within the deeper low-oxygen layer. Combined with the existence of steep geochemical gradients, the introduction of a favorable manganese oxide oxidant from the upper oxic layer into the underlying low oxygen region during diffusive mixing resulted in the higher concentrations of nitrate observed (due to the anoxic reoxidation of nitrite to nitrate) as well as the strong positive correlation of nitrite/nitrate with manganese (II) ion concentrations (in the deeper anoxic layer compared with the shallower oxic layer). The observations and findings presented herein have implications for not only reconciling the discrepancies in such unconventional pathways of nitrogen metabolism between groundwater ecosystems and river/stream/-soil/marine systems (where such processes have most commonly been reported) but also for devising effective nitrogen nutrient remediation and complex nitrogen-cycling modeling strategies.

Hydrological extremes can affect nutrient export from catchments to streams, posing a threat to aquatic ecosystems. In this study, we investigated the effects of hydrological drought on nitrate concentrations in the streamflow of 182 German catchments from 1980 to 2020. We found that across all seasons, 40% and 25% of the catchments showed significantly lower nitrate concentrations during drought and post-droughts, respectively, when compared to non-drought conditions. However, we observed pronounced spatial variability in the responses, particularly during winter droughts and post-droughts, with more catchments exhibiting higher nitrate concentrations. Specifically, nitrate concentrations were significantly higher in 25% of the study catchments during winter droughts, particularly in wetter catchments with low nitrogen retention. During winter post-droughts, nitrate concentrations are significantly higher in 19% of the catchments, especially in wetter catchments with more nitrogen surplus. Moreover, the likelihood of nitrate seasonal extremes increased by 6% during winter post-drought in our study catchments. Considering the projected increase in the frequency of droughts in Germany, the increase in nitrate concentrations during the corresponding post-drought periods poses a potential threat to aquatic ecosystem health.

To study the significance of land use and catchment hydrology for the age of exported carbon, we measured the radiocarbon abundances in two mountainous streams in Germany. The Hassel catchment was characterized by wider-stretched riparian areas and by a significant contribution of arable land and pasture to land use compared to the Rappbode catchment. Although soil cultivation is considered to mobilize old carbon from deep soil layers, in six out of eight situations dissolved organic carbon (DOC) was younger in Hassel stream compared to Rappbode. In contrast, we estimated annual exports of radiocarbon on the basis of yield weighed, bulked biweekly samples and found that older DOC was delivered from Hassel compared to Rappbode catchment (352 years conventional radiocarbon age as well as carbon near to modern origin, respectively). This result characterized primarily the fluxes during wet conditions, which dominated the annual exports. In a winter base flow situation, we found that old (~2550 years) snow-bound organic carbon deriving from atmospheric deposition contributed 29–43 % to stream exports. Overall, there was significant intra-annual variability of stream ¹⁴C-DOC. Within the catchments, the standard deviations of ∆¹⁴C values (47–63 ‰) were comparable to the difference of annual exports between the contrasting catchments (46 ‰). Infrequent storm flow events should be included not only in export budgets but also in studies of carbon sources.

The paper presents an improved approach for investigating submarine groundwater discharge (SGD) based on radon mapping and radon mass balancing in the coastal sea. While the use of radon as an environmental tracer in SGD studies is well-established, we identified based on our longstanding experience six methodical shortcomings of the conventional approach and suggest corresponding developments. The shortcomings include: (1 and 2) inadequate consideration of both detection equipment response delay and influence of tidal stage; (3 and 4) incorrect quantification of radon losses, due to offshore mixing and degassing resulting in a potentially incorrect radon mass balance; (5) inaccurate determination of the terrestrial groundwater endmember, due to inhomogeneous radon distribution in the coastal aquifer; and (6) difficulties in distinguishing between discharged fresh groundwater and recirculated seawater. The improved approach is practically demonstrated in a step by step manner in a large-scale field study, which was carried out in False Bay (South Africa) and which consisted of two parts, namely (i) qualitative SGD localization along the entire False Bay coastline based on coastal radon distribution patterns and (ii) quantitative SGD investigation within a defined coastal area of interest (AOI) based on a radon mass balance (RMB). The plausibility of the AOI related results was evaluated by a hydrogeological model, used for qualitative SGD localization, and a hydrological model, applied for estimating groundwater recharge within the AOI catchment.

Purpose The present study investigated lake and river sediments affected by metals from an acid mine drainage (AMD) from a former uranium mine. The role of bacterial sulfate reduction in the immobilization of contaminants was evaluated, and the analyses of acid volatile sulfide (AVS) and sequential extraction were performed. Consequently, the potential mobility and bioavailability of contaminants were established. Materials and methods Sulfur isotopic fractionation (δ 34 S), AVS, and sequential extraction procedure were used to assess the sulfate bacterial reduction and the availability of contaminants in the environment at six sampling stations. Results and discussion The δ 34 S indicated that bacterial reduction is a key process in the natural attenuation of contamination in the Águas Claras reservoir, precipitating metal sulfides. According to the USEPA criteria, adverse biological effects are expected for sample S1 (inside the reservoir) which is likely to be toxic, while for sediment S4 (in the river), the toxicity is uncertain. The other samples were classified as non-toxic, likely because of the decreased solubility of zinc sulfide. A decrease in the concentration of the contaminants downstream of the reservoir was observed. The predominance of U (0.4 %) in the labile fraction and the elevated concentrations of Zn (0.5 %) and Mn (0.7 %) in the sediments inside the reservoir raises concerns regarding the availability of these contaminants in the environment. Conclusions The main environmental impact appears to be concentrated in the Águas Claras reservoir, whereas the Antas creek does not seem to be affected by the AMD process. Although the bacterial sulfate reduction is effective in its production of sulfides capable of immobilizing the contaminants, the presence of Zn and U in the labile and reducible fraction is a matter of concern due to its long-term bioavailability. Thus, continuous monitoring of the redox potential of the waters and sediments, mainly in the reservoir, is recommended in order to assess and possibly prevent later dissolution of sequestered contaminants.

Soluble reactive phosphorus (SRP) concentrations in agricultural headwaters can display pronounced seasonal variability at low flow, often with the highest concentrations occurring in summer. These SRP concentrations often exceed eutrophication levels, but their main sources, spatial distribution, and temporal dynamics are often unknown. The purpose of this study is therefore to differentiate between potential SRP losses and releases from soil drainage, anoxic riparian wetlands, and stream sediments in an agricultural headwater catchment. To identify the dominant SRP sources, we carried out three longitudinal stream sampling campaigns for SRP concentrations and fluxes. We used salt dilution tests and natural 222Rn to determine water fluxes in different sections of the stream, and we sampled for SRP, Fe, and 14C dissolved organic carbon (DOC) to examine possible redox-mediated mobilization from riparian wetlands and stream sediments. The results indicate that a single short section in the upper headwater reach was responsible for most of the SRP fluxes to the stream. Analysis of samples taken under summer low-flow conditions revealed that the stream water SRP concentrations, the fraction of SRP within total dissolved P (TDP), and DOC radiocarbon ages matched those in the groundwater entering the gaining section. Pore water from the stream sediment showed evidence of reductive mobilization of SRP, but the exchange fluxes were probably too small to contribute substantially to SRP stream concentrations. We also found no evidence that shallow flow paths from riparian wetlands contributed to the observed SRP loads in the stream. Combined, the results of this campaign and previous monitoring suggest that groundwater is the main long-term contributor of SRP at low flow, and agricultural phosphorus is largely buffered in the soil zone. We argue that the seasonal variation of SRP concentrations was mainly caused by variations in the proportion of groundwater present in the streamflow, which was highest during summer low-flow periods. Accurate knowledge of the various input pathways is important for choosing effective management measures in a given catchment, as it is also possible that observations of seasonal SRP dilution patterns stem from increased mobilization in riparian zones or from point sources.

Information about groundwater residence times is essential for sustainable groundwater management. Naturally occurring radionuclides are suitable tools for related investigations. While the applicability of several long-lived radionuclides has been demonstrated for the investigation of long residence times (i.e., years, decades, centuries and more), studies that focus on sub-yearly residence times are only scarcely discussed in the literature. This shortage is mainly due to the rather small number of radionuclides that are generally suitable for the purpose and show at the same time adequately short half-lives. A promising innovative approach in this regard applies cosmogenic radiosulfur ([sup.35]S). [sup.35]S is continuously produced in the stratosphere from where it is conveyed to the troposphere or lower atmosphere and finally transferred with the rain to the groundwater. As soon as the meteoric water enters the subsurface, its [sup.35]S activity decreases with an 87.4 day half-life, making [sup.35]S a suitable time tracer for investigating sub-yearly groundwater ages. However, since precipitation shows a varying [sup.35]S activity during the year, setting up a reliable [sup.35]S input function is required for sound data evaluation. That calls for (i) an investigation of the long-term variation of the [sup.35]S activity in the rain, (ii) the identification of the associated drivers and (iii) an approach for setting up a [sup.35]S input function based on easily attainable proxies. The paper discusses [sup.35]S activities in the rain recorded over a 12-month period, identifies natural and anthropogenic influences, and suggests an approach for setting up a [sup.35]S input function applying [sup.7]Be as a proxy.

This article provides an overview about the Bode River catchment that was selected as the hydrological observatory and main region for hydro-ecological research within the TERrestrial ENvironmental Observatories Harz/Central German Lowland Observatory. It first provides information about the general characteristics of the catchment including climate, geology, soils, land use, water quality and aquatic ecology, followed by the description of the interdisciplinary research framework and the monitoring concept with the main components of the multi-scale and multi-temporal monitoring infrastructure. It also shows examples of interdisciplinary research projects aiming to advance the understanding of complex hydrological processes under natural and anthropogenic forcings and their interactions in a catchment context. The overview is complemented with research work conducted at a number of intensive research sites, each focusing on a particular functional zone or specific components and processes of the hydro-ecological system.

In batch experiments, we studied the isotope fractionation of nitrogen and oxygen during denitrification of two bacterial strains (Azoarcus sp. strain DSM 9056 and Pseudomonas pseudoalcaligenes strain F10). Denitrification experiments were conducted with succinate and toluene as electron donor in three waters with a distinct oxygen isotope composition. Nitrate consumption was observed in all batch experiments. Reaction rates for succinate experiments were more than six times higher than those for toluene experiments. Nitrogen and oxygen isotopes became progressively enriched in the remaining nitrate pool in the course of the experiments; the nitrogen and oxygen isotope fractionation varied between 8.6-16.2 and 4.0-7.3‰, respectively. Within this range, neither electron donors nor the oxygen isotope composition of the medium affected the isotope fractionation process. The experimental results provide evidence that the oxygen isotope fractionation during nitrate reduction is controlled by a kinetic isotope effect which can be quantified using the Rayleigh model. The isotopic examination of nitrite released upon denitrification revealed that nitrogen isotope fractionation largely follows the fractionation of the nitrate pool. However, the oxygen isotope values of nitrite are clearly influenced by a rapid isotope equilibration with the oxygen of the ambient water. Even though this equilibration may in part be due to storage, it shows that under certain natural conditions (re-oxidation of nitrite) the nitrate pool may also be indirectly affected by an isotope equilibration.