Combined Surface-Subsurface Stream Restoration Structures Can Optimize Hyporheic Attenuation of Stream Water Contaminants.

There is a design-to-function knowledge gap regarding how engineered stream restoration structures can maximize hyporheic contaminant attenuation. Surface and subsurface structures have each been studied in isolation as techniques to restore hyporheic exchange, but surface-subsurface structures have not been investigated or optimized in an integrated manner. Here, we used a numerical model to systematically evaluate key design variables for combined surface (i.e., weir height and length) and subsurface (i.e., upstream and downstream baffle plate spacing) structures. We also compared performance metrics that place differing emphasis on hyporheic flux versus transit times. We found that surface structures tended to create higher flux, shorter transit time flowpaths, whereas subsurface structures promoted moderate-flux, longer transit time flowpaths. Optimal combined surface-subsurface structures could increase fluxes and transit times simultaneously, thus providing conditions for contaminant attenuation that were many times more effective than surface or subsurface structures alone. All performance metrics were improved by the presence of an upstream plate and the absence of a downstream plate. Increasing the weir length tended to improve all metrics, whereas the optimal weir height varied based on metrics. These findings may improve stream restoration by better aligning specific restoration goals with appropriate performance metrics and hyporheic structure designs.

Flow and Transport Modeling in Heterogeneous Sediments Using an Integral Approach.

An integral approach which can simultaneously model turbulent flow and transport at the sediment-water interface has been recently developed and validated for homogeneous sediment which was achieved by comparing numerical results to flume experiments on flow and transport over a rippled streambed and through the sediment for neutral, gaining, and losing conditions. In the present study, we validated the approach for heterogeneous conditions by comparing numerical simulations of flow and transport in heterogeneous sediment to analytical solutions as well as flume experiments on flow and transport through rippled streambed consisting of heterogeneous sediment. For this complex setup, simulation and experimental results agree well showing that flow and tracer transport prefer paths through areas with bigger grain diameters and higher porosities. The effect of flow redirections under losing and gaining conditions on hyporheic flow and residence times is discussed.

Fate of trace organic compounds in the hyporheic zone: Influence of microbial metabolism.

The hyporheic zone (HZ) is considered a hydrodynamically-driven bioreactor with significant pollutant removal capacities and can therefore not only improve wholestream water quality but also preserve human and ecosystem health. Microbial metabolism is hypothesized to play a key role in pollutant transformation in hyporheic sediments of natural streams. However, previous work investigating the influence of microbial metabolism on pollutant transformation has been predominantly laboratory studies. The key challenge for field studies is the appropriate determination of net microbial metabolism, i.e. information on the actual exposure times to specific microbial processes in the investigated system. The present study uses reactive fluorescent tracers to determine microbial metabolism and ultimately its influence on pollutant transformation, e.g. for trace organic compounds, in hyporheic sediments under natural conditions. In particular, the reactive fluorescent tracers resazurin and its main transformation product resorufin were used to determine the microbial metabolism of facultative or obligate aerobes. The influence of the derived microbial metabolism on the transformation of 20 trace organic compounds, such as pharmaceuticals, including 3 parent-daughter pairs, was examined. The present findings validate laboratory results on the microbially-mediated transformation of the anticonvulsant gabapentin to its main transformation product gabapentin lactam under natural conditions. All other TrOCs investigated did not show a clear link between TrOC reactivity to the microbial metabolism informed by the resazurin-resorufin-system. Overall, the present study not only demonstrates the use of the fluorescent tracer-system resazurin and resorufin for determining microbial metabolism of facultative or obligate aerobes but also generally highlights the potential of reactive fluorescent tracers to disentangle specific reactive properties and ultimately their influence on the fate of pollutants in natural HZs.

Determining hyporheic removal rates of trace organic compounds using non-parametric conservative transport with multiple sorption models.

Assessing the transport and reactive processes of contaminants in freshwater streams is crucial in managing water resources sustainably. Particularly the hyporheic zone, the sediment-water interface where surface water and groundwater mix, may possess significant contaminant removal capacities due to its myriad physical, chemical, and microbiological processes. However, modelling approaches aiming at assessing the hyporheic zone's reactivity are either based on simple assumptions, such as, predefining the shape of the residence times distribution (RTD) function, or are computationally not feasible due to a too detailed system characterisation. In addition, parent-daughter reactions of contaminants are barely investigated. The present study introduces a numerical modelling framework for assessing hyporheic reactions of contaminant transformation reactions based on a non-parametric residence time approach combined with multiple sorption models and first-order removal reactions. The proposed framework uses natural electrical conductivity fluctuations to determine conservative transport properties and is demonstrated by interpreting time series of hyporheic point measurements of trace organic compounds, such as pharmaceuticals, and their transformation products using two commonly-used sorption models, namely the simple retardation and the first-order kinetic sorption model. The developed approach gives similar reaction rate coefficient estimates for all contaminants considered for both sorption models tested. The findings highlight that (i) the accurate shape of the RTD is most certainly important for reactive parameter determination and (ii) the daughter reaction rate coefficient may be underestimated if its parent transformation is ignored. The model provides reactive parameter estimates of contaminant transformation reactions with high parameter identifiability and informs which specific parent-daughter-pathway has occurred.

Transformation of organic micropollutants along hyporheic flow in bedforms of river-simulating flumes.

Urban streams receive increasing loads of organic micropollutants from treated wastewaters. A comprehensive understanding of the in-stream fate of micropollutants is thus of high interest for water quality management. Bedforms induce pumping effects considerably contributing to whole stream hyporheic exchange and are hotspots of biogeochemical turnover processes. However, little is known about the transformation of micropollutants in such structures. In the present study, we set up recirculating flumes to examine the transformation of a set of micropollutants along single flowpaths in two triangular bedforms. We sampled porewater from four locations in the bedforms over 78 days and analysed the resulting concentration curves using the results of a hydrodynamic model in combination with a reactive transport model accounting for advection, dispersion, first-order removal and retardation. The four porewater sampling locations were positioned on individual flowpaths with median solute travel times ranging from 11.5 to 43.3 h as shown in a hydrodynamic model previously. Highest stability was estimated for hydrochlorothiazide on all flowpaths. Lowest detectable half-lives were estimated for sotalol (0.7 h) and sitagliptin (0.2 h) along the shortest flowpath. Also, venlafaxine, acesulfame, bezafibrate, irbesartan, valsartan, ibuprofen and naproxen displayed lower half-lives at shorter flowpaths in the first bedform. However, the behavior of many compounds in the second bedform deviated from expectations, where particularly transformation products, e.g. valsartan acid, showed high concentrations. Flowpath-specific behavior as observed for metformin or flume-specific behavior as observed for metoprolol acid, for instance, was attributed to potential small-scale or flume-scale heterogeneity of microbial community compositions, respectively. The results of the study indicate that the shallow hyporheic flow field and the small-scale heterogeneity of the microbial community are major controlling factors for the transformation of relevant micropollutants in river sediments.

High-Resolution Integrated Transport Model for Studying Surface Water-Groundwater Interaction.

Transport processes that lead to exchange of mass between surface water and groundwater play a significant role for the ecological functioning of aquatic systems, for hydrological processes and for biogeochemical transformations. In this study, we present a novel integral modeling approach for flow and transport at the sediment-water interface. The model allows us to simultaneously simulate turbulent surface and subsurface flow and transport with the same conceptual approach. For this purpose, a conservative transport equation was implemented to an existing approach that uses an extended version of the Navier-Stokes equations. Based on previous flume studies which investigated the spreading of a dye tracer under neutral, losing and gaining flow conditions the new solver is validated. Tracer distributions of the experiments are in close agreement with the simulations. The simulated flow paths are significantly affected by in- and outflowing groundwater flow. The highest velocities within the sediment are found for losing condition, which leads to shorter residence times compared to neutral and gaining conditions. The largest extent of the hyporheic exchange flow is observed under neutral condition. The new solver can be used for further examinations of cases that are not suitable for the conventional coupled models, for example, if Reynolds numbers are larger than 10. Moreover, results gained with the integral solver provide high-resolution information on pressure and velocity distributions at the rippled streambed, which can be used to improve flow predictions. This includes the extent of hyporheic exchange under varying ambient groundwater flow conditions.

Bacterial Diversity Controls Transformation of Wastewater-Derived Organic Contaminants in River-Simulating Flumes.

Hyporheic zones are the water-saturated flow-through subsurfaces of rivers which are characterized by the simultaneous occurrence of multiple physical, biological, and chemical processes. Two factors playing a role in the hyporheic attenuation of organic contaminants are sediment bedforms (a major driver of hyporheic exchange) and the composition of the sediment microbial community. How these factors act on the diverse range of organic contaminants encountered downstream from wastewater treatment plants is not well understood. To address this knowledge gap, we investigated dissipation half-lives (DT50s) of 31 substances (mainly pharmaceuticals) under different combinations of bacterial diversity and bedform-induced hyporheic flow using 20 recirculating flumes in a central composite face factorial design. By combining small-volume pore water sampling, targeted analysis, and suspect screening, along with quantitative real-time PCR and time-resolved amplicon Illumina MiSeq sequencing, we determined a comprehensive set of DT50s, associated bacterial communities, and microbial transformation products. The resulting DT50s of parent compounds ranged from 0.5 (fluoxetine) to 306 days (carbamazepine), with 20 substances responding significantly to bacterial diversity and four to both diversity and hyporheic flow. Bacterial taxa that were associated with biodegradation included Acidobacteria (groups 6, 17, and 22), Actinobacteria (Nocardioides and Illumatobacter), Bacteroidetes (Terrimonas and Flavobacterium) and diverse Proteobacteria (Pseudomonadaceae, Sphingomonadaceae, and Xanthomonadaceae). Notable were the formation of valsartan acid from irbesartan and valsartan, the persistence of N-desmethylvenlafaxine across all treatments, and the identification of biuret as a novel transformation product of metformin. Twelve additional target transformation products were identified, which were persistent in either pore or surface water of at least one treatment, indicating their environmental relevance.

The method controls the story - Sampling method impacts on the detection of pore-water nitrogen concentrations in streambeds.

Biogeochemical gradients in streambeds are steep and can vary over short distances often making adequate characterisation of sediment biogeochemical processes challenging. This paper provides an overview and comparison of streambed pore-water sampling methods, highlighting their capacity to address gaps in our understanding of streambed biogeochemical processes. This work reviews and critiques available pore-water sampling techniques to characterise streambed biogeochemical conditions, including their characteristic spatial and temporal resolutions, and associated advantages and limitations. A field study comparing three commonly-used pore-water sampling techniques (multilevel mini-piezometers, miniature drivepoint samplers and diffusive equilibrium in thin-film gels) was conducted to assess differences in observed nitrate and ammonium concentration profiles. Pore-water nitrate concentrations did not differ significantly between sampling methods (p-value = 0.54) with mean concentrations of 2.53, 4.08 and 4.02 mg l-1 observed with the multilevel mini-piezometers, miniature drivepoint samplers and diffusive equilibrium in thin-film gel samplers, respectively. Pore-water ammonium concentrations, however, were significantly higher in pore-water extracted by multilevel mini-piezometers (3.83 mg l-1) and significantly lower where sampled with miniature drivepoint samplers (1.05 mg l-1, p-values <0.01). Differences in observed pore-water ammonium concentration profiles between active (suction: multilevel mini-piezometers) and passive (equilibrium; diffusive equilibrium in thin-film gels) samplers were further explored under laboratory conditions. Measured pore-water ammonium concentrations were significantly greater when sampled by diffusive equilibrium in thin-film gels than with multilevel mini-piezometers (all p-values ≤0.02). The findings of this study have critical implications for the interpretation of field-based research on hyporheic zone biogeochemical cycling and highlight the need for more systematic testing of sampling protocols. For the first time, the impact of different active and passive pore-water sampling methods is addressed systematically here, highlighting to what degree the choice of pore-water sampling methods affects research outcomes, with relevance for the interpretation of previously published work as well as future studies.

The effect of unsteady streamflow and stream-groundwater interactions on oxygen consumption in a sandy streambed.

Streamflow dynamics are often ignored when studying biogeochemical processes in the hyporheic zone. We explored the interactive effects of unsteady streamflow and groundwater fluxes on the delivery and consumption of oxygen within the hyporheic zone using a recirculating flume packed with natural sandy sediments. The flume was equipped with a programmable streamflow control and drainage system that was used to impose losing and gaining fluxes. Tracer tests were used to measure hyporheic exchange flux and a planar optode was used to measure subsurface oxygen concentration patterns. It was found that the volume of the oxic zone decreased when the losing flux declined, and was drastically decreased when gaining conditions were applied. It was also found that unsteady streamflow led to a slight increase in the average volume of the oxic zone, compared to the average volume of the oxic zone under steady streamflow. However, the average oxygen consumption rates were significantly higher under unsteady streamflow compared to steady streamflow under all groundwater conditions with the exception of the highest losing flux. The present study provides the first insight into the interactions between streamflow unsteadiness and losing/gaining fluxes and improve understanding of their impact on microbial metabolism in the hyporheic zone.

Author Correction: Environmental filtering and community delineation in the streambed ecotone.

A correction to this article has been published and is linked from the HTML and PDF versions of this paper. The error has been fixed in the paper.

Chironomid larvae enhance phosphorus burial in lake sediments: Insights from long-term and short-term experiments.

Tube-dwelling macrozoobenthos can affect lake ecosystems in myriad ways, including changes in nutrient fluxes across the sediment-water interface. The pumping activity of chironomid larvae reinforces the transport of solutes between sediment and water. The transport of oxygen into the area surrounding the burrows generates oxidized compounds such as iron(oxy)hydroxides, which results in an additional phosphorus (P) sorption capacity similar to that of oxidized sediment surfaces. In the present study, the effect of the oxidized burrow walls of Chironomus plumosus on P binding capacity and P binding forms was tested in the laboratory using sediments with differing iron contents and varying numbers of chironomid larvae. In an additional long-term experiment, lake sediment naturally rich in iron was incubated under oxic conditions for 165 days, followed by a 3.5-year anoxic period. These experiments showed that: (1) Under oxic conditions the cumulative P uptake by sediments was dependent on larval densities. (2) The P that accumulated both at the sediment-water interface and in the oxidized burrow walls was mainly present as reductive soluble P (iron-bound P). Surprisingly, the amount of P released during the anoxic period in the long-term experiment was independent of the amount of P previously taken up during the oxic period since a portion of P was permanently retained in the sediment. The increase in alkaline soluble metal-bound P (NaOH-SRP) in formerly colonized sediments is a strong indication that the excessive P fixation by reductive soluble iron triggers the subsequent formation of stable iron phosphate minerals such as vivianite. Our study shows that P fixation that is induced by chironomid larvae is not always a completely reversible phenomenon, even after the emergence of the larvae and the re-establishment of anoxic conditions in the sediment.

Environmental filtering and community delineation in the streambed ecotone.

A current controversy in ecology is whether biological communities are discrete biological entities or simply study units created for convenience; a debate that becomes even more heated when delimiting communities along ecotones. Here, we report an interdisciplinary study designed to address the interplay between environmental drivers and community ecology in a typical ecotone ecosystem: the streambed. Environmental filtering at a micro-scale determined how diversity, productivity and composition of the whole streambed assemblage varied with depth and with the direction of vertical water exchange. Biomass and production decreased with increasing depth, and were lower under upwelling than downwelling conditions. However, the rate at which biomass and production decreased with increasing depth differed significantly for different taxonomic groups. Using quantitative biocenosis analysis, we also showed that benthic and hyporheic zone assemblages (assemblages in close juxtaposition) could be clearly distinguished as discrete communities with individual integrity. Vertical hydrodynamic conditions also influenced the demarcation between both communities; the benthic community reached greater depths in downwelling than in upwelling zones.

The fate of polar trace organic compounds in the hyporheic zone.

The hyporheic zone (HZ) is often considered to efficiently remove polar trace organic compounds (TrOCs) from lotic systems, mitigating potential adverse effects of TrOCs on ecosystem functioning and drinking water production. Predicting the fate of TrOCs in the hyporheic zone (HZ) is difficult as the in-situ removal rate constants are not known and the biogeochemical factors as well as hydrological conditions controlling the removal efficiency are not fully understood. To determine the in-situ removal efficiency of the HZ for a variety of TrOCs as a function of the biogeochemical milieu, we conducted a field study in an urban river near Berlin, Germany. Subsurface flow was studied by time series of temperature depth profiles and the biogeochemical milieu of the HZ by concentration depth profiles. These results, in conjunction with a 1D advection-dispersion transport model, were used to calculate first-order removal rate constants of several polar TrOCs in the HZ. For the majority of TrOCs investigated, removal rate constants were strongly dependent on redox conditions, with significantly higher removal rates observed under predominantly suboxic (i.e. denitrifying) compared to anoxic (i.e. Fe and Mn reducing) conditions. Compared to previous studies on the fate of TrOCs in saturated sediments, half-lives within oxic/suboxic sections of the HZ were relatively low, attributable to the site-specific characteristics of the HZ in a stream dominated by wastewater treatment plant effluent. For nine out of thirteen investigated TrOCs, concentrations decreased significantly in the HZ with relative removal percentages ranging from 32% for primidone to 77% for gabapentin. For many TrOCs, removal efficiency decreased drastically as redox conditions became anoxic. For the majority of compounds investigated here, the HZ indeed acts as an efficient bioreactor that is capable of removing TrOCs along relatively short flow paths. Depending on the TrOC, removal capacity may be enhanced by either increasing the magnitude of groundwater-surface exchange fluxes, by increasing the total residence time in the HZ or the exposure time to suboxic zones, respectively.

Bioturbation enhances the aerobic respiration of lake sediments in warming lakes.

While lakes occupy less than 2% of the total surface of the Earth, they play a substantial role in global biogeochemical cycles. For instance, shallow lakes are important sites of carbon metabolism. Aerobic respiration is one of the important drivers of the carbon metabolism in lakes. In this context, bioturbation impacts of benthic animals (biological reworking of sediment matrix and ventilation of the sediment) on sediment aerobic respiration have previously been underestimated. Biological activity is likely to change over the course of a year due to seasonal changes of water temperatures. This study uses microcosm experiments to investigate how the impact of bioturbation (by Diptera, Chironomidae larvae) on lake sediment respiration changes when temperatures increase. While at 5°C, respiration in sediments with and without chironomids did not differ, at 30°C sediment respiration in microcosms with 2000 chironomids per m(2) was 4.9 times higher than in uninhabited sediments. Our results indicate that lake water temperature increases could significantly enhance lake sediment respiration, which allows us to better understand seasonal changes in lake respiration and carbon metabolism as well as the potential impacts of global warming.

Effects of bioirrigation of non-biting midges (Diptera: Chironomidae) on lake sediment respiration.

Bioirrigation or the transport of fluids into the sediment matrix due to the activities of organisms such as bloodworms (larvae of Diptera, Chironomidae), has substantial impacts on sediment respiration in lakes. However, previous quantifications of bioirrigation impacts of Chironomidae have been limited by technical challenges such as the difficulty to separate faunal and bacterial respiration. This paper describes a novel method based on the bioreactive tracer resazurin for measuring respiration in-situ in non-sealed systems with constant oxygen supply. Applying this new method in microcosm experiments revealed that bioirrigation enhanced sediment respiration by up to 2.5 times. The new method is yielding lower oxygen consumption than previously reported, as it is only sensitive to aerobic heterotrophous respiration and not to other processes causing oxygen decrease. Hence it decouples the quantification of respiration of animals and inorganic oxygen consumption from microbe respiration in sediment.

Long-term efficiency of lake restoration by chemical phosphorus precipitation: Scenario analysis with a phosphorus balance model.

An artificial increase of phosphorus (P) retention in lakes with a long residence time and/or a large mobile sediment P pool by adding P binding chemicals can drastically shorten the time these lakes require to reach water quality targets. Suitable tools to optimize timing and extent of external and internal measures are lacking. The one-box model, a mass balance tool for predicting the P trend in the water under different management options was applied to highly eutrophic Lake Arendsee (a = 5.14 km(2), zmax = 49 m), Germany. Mass developments of blue green algae and increasing hypolimnetic oxygen deficiencies are urgent reasons for restoring Lake Arendsee. Detailed studies of P cycling and scenario analyses with the one-box model led to the following conclusions: i) immediate improvement of the trophic state is only possible by in-lake P inactivation because of the long water residence time (56 years); ii) a gradual external P load reduction, even if the effect is delayed, will assure the sustainability of the scheduled Al application beyond one decade; iii) a twofold precipitation reduces the risk of failure compared to a singular application with an overdose related to the relevant internal P pools.

Investigating groundwater-lake interactions by hydraulic heads and a water balance.

Discharge of groundwater into lakes (lacustrine groundwater discharge, LGD) can play a major role in water balances of lakes. Unfortunately, studies often neglect this input path because of methodological difficulties in its determination. Direct measurements of LGD are labor-consuming and prone to error. The present study uses both spatially variable hydraulic-head data and meteorological data to estimate groundwater input by LGD and lake water output through infiltration. The study sites are two shallow, groundwater-fed lakes without any surface inflows or outflows. Horizontally interpolated groundwater heads were combined with lake water levels to obtain vertical hydraulic gradients between the aquifer and the lake, which are separated by a thick layer of lake bed sediment which has a much lower hydraulic conductivity than the underlying aquifer. By fitting the hydraulic gradient to the results of a simple mass balance and considering the process of clogging, we were able to estimate the hydraulic conductivity of the lake bed sediments. We calculated groundwater inputs by LGD and lake water outputs by infiltration on an annual basis. Although our method requires several assumptions, the results are reasonable and provide useful information about the exchange between the aquifer and the lake, which can, for example, be used for the calculation of nutrient mass balances.

Fate of organic micropollutants in the hyporheic zone of a eutrophic lowland stream: results of a preliminary field study.

Many rivers and streams worldwide are impacted by pharmaceuticals originating from sewage. The hyporheic zone underlying streams is often regarded as reactive bioreactor with the potential for eliminating such sewage-born micropollutants. The present study aims at checking the elimination potential and analyzing the coupling of hydrodynamics, biogeochemistry and micropollutant processing. To this end, two sites at the lowland stream Erpe, which receives a high sewage burden, were equipped and sampled with nested piezometers. From temperature depth profiles we determined that at one of the sites infiltration of surface water into the aquifer occurs while exfiltration dominates at the other site. Biogeochemical data reveal intense mineralization processes and strictly anoxic conditions in the streambed sediments at both sites. Concentrations of the pharmaceuticals indomethacin, diclofenac, ibuprofen, bezafibrate, ketoprofen, naproxen and clofibric acid were high in the surface water and also in the subsurface at the infiltrating site. The evaluation of the depth profiles indicates some attenuation but due to varying surface water composition the evaluation of subsurface processes is quite complex. Borate and non-geogenic gadolinium were measured as conservative wastewater indicators. To eliminate the influence of fluctuating sewage proportions in the surface water, micropollutant concentrations are related to these indicators. The indicators can cope with different dilutions of the sewage but not with temporally varying sewage composition.