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In situ bioremediation is a common remediation strategy for many groundwater contaminants. It was traditionally believed that (in the absence of mixing-limitations) a better in situ bioremediation is obtained in a more homogeneous medium where the even distribution of both substrate and bacteria facilitates the access of a larger portion of the bacterial community to a higher amount of substrate. Such conclusions were driven with the typical assumption of disregarding substrate inhibitory effects on the metabolic activity of enzymes at high concentration levels. To investigate the influence of pore matrix heterogeneities on substrate inhibition, we use a numerical approach to solve reactive transport processes in the presence of pore-scale heterogeneities. To this end, a rigorous reactive pore network model is developed and used to model the reactive transport of a self-inhibiting substrate under both transient and steady-state conditions through media with various, spatially correlated, pore-size distributions. For the first time, we explore on the basis of a pore-scale model approach the link between pore-size heterogeneities and substrate inhibition. Our results show that for a self-inhibiting substrate, (1) pore-scale heterogeneities can consistently promote degradation rates at toxic levels, (2) the effect reverses when the concentrations fall to levels essential for microbial growth, and (3) an engineered combination of homogeneous and heterogeneous media can increase the overall efficiency of bioremediation.

Understanding phosphorus (P) dynamics in urban landscapes is an emerging research topic as P export from urban landscapes towards aquatic ecosystems causes eutrophication-related challenges in these environments. We investigated P export and forms in four research sites in Ontario, Canada, including three urban catchments and a stormwater pond, all located within the Great Toronto Area in the drainage basin of Lake Ontario. We conducted P speciation laboratory analyses on runoff and suspended sediment samples to measure total P (TP), total dissolved P (TDP), dissolved reactive P (DRP), dissolved unreactive P (TDP–DRP), and PP (TP–TDP). Multiple linear regression (MLR) models were also developed to quantify annual loadings of these P species. Models indicated that P loadings in our sites were close to the lower limit of values reported in the literature, with the simulated range of 0.2—0.46 kg ha-1 yr-1 for TP export, 0.06—0.168 kg ha-1 yr-1 for TDP, 0.011—0.073 kg ha-1 yr-1 for DRP, 0.026—0.095 kg ha-1 yr-1 for DUP, and 0.163—0.288 kg ha-1 yr-1 for PP. In our MLR models, precipitation explained a large fraction of variability in loadings with the median of 58% across all models. Moreover, we realized that as the proportion of residential land within the drainage area increased, larger amounts of P loadings were exported at the catchment scale. Results also implied that pond served as a major P sink, with annual retention of 82, 93, 91, 94, and 77% for TP, TDP, DRP, DUP, and PP, respectively. Mass balance analyses based on sequential P extraction in the sediment core samples revealed that P retention was attributed to sedimentation in the ponds, as well as chemical precipitation of P with calcium mineral phases. In terms of P composition, most of P export in our sites (72—88%) were in particulate form. Besides, the ratio between dissolved forms and TP were the highest in the catchment with the largest amount green spaces. This study demonstrates that, as land-use characteristics impose variations in constituent loadings, urban P management options also have to be varying from a catchment to another. However, sediment removing practices such as the use of ponds will certainly be a reliable P retention approach as most of urban P could be sediment-bound. Furthermore, enhancing the formation of calcium phosphate and other redox-stable mineral phases could be explored as a best management practice in existing and new ponds for improving P retention.

Economic valuations of ecosystem services often transfer previously estimated global unit values to the geographical setting of interest. While this approach produces quick results, its reliability depends on how representative the large-scale average unit values are for the given local context. Here, we estimate the values of three ecosystem services (ES) – water filtration, nutrient cycling and carbon sequestration – in the Grand River watershed (GRW) of southern Ontario, Canada. The watershed covers nearly 7000 km2, has a humid continental climate and a population of close to one million people. Land cover is dominated by agriculture. We compare ES valuations using locally derived (i.e., GRW-specific) unit values to valuations based on unit values from a regional database and those compiled in the global Ecosystem Services Valuation Database (ESVD). The regional database includes mean unit values from three case studies within southern Ontario and one boreal watershed in British Columbia. As expected, the regional database yields average monetary values for the three ES that are close to those obtained with the local unit values but with larger associated uncertainties. Using the ESVD, however, results in significantly higher monetary values for the ES. For water filtration, the ESVD value is more than five times higher than the regional and local estimates. We further illustrate the effect of the extent of aggregation of forested and agricultural land categories on the ES values. For example, by subdividing the forest category into three sub-categories (deciduous, coniferous, and mixed forest), the estimated value of the carbon sequestration ES of forested areas within the GRW increases by 15%. Overall, our results emphasize the importance of critically assessing the origin of unit values and the land cover resolution in ES valuation, especially when the latter is used as a policy-guiding tool.

Increasing incidences of eutrophication and groundwater quality impairment from agricultural nitrogen pollution are threatening humans and ecosystem health. Minimal improvements in water quality have been achieved despite billions of dollars invested in conservation measures worldwide. Such apparent failures can be attributed in part to legacy nitrogen that has accumulated over decades of agricultural intensification and that can lead to time lags in water quality improvement. Here, we identify the key knowledge gaps related to landscape nitrogen legacies and propose approaches to manage and improve water quality, given the presence of these legacies.

Microbial degradation of organic matter is a key driver of subsurface biogeochemistry. Here, we present a bioenergetics-informed kinetic model for the anaerobic degradation of macromolecular organic matter that accounts for extracellular hydrolysis, fermentation, and respiration. The catabolic energy generated by fermentation and respiration is allocated to biomass growth, production of extracellular hydrolytic enzymes, and cellular maintenance. Microbial cells are assumed to exist in active or dormant states with marked differences in maintenance energy requirements. Dormant cells are further assumed to fulfill their maintenance energy requirements by utilizing their own biomass instead of relying on external substrates. When the catabolic Gibbs energy production for a given functional group of microorganisms exceeds the total maintenance energy requirement of the active cells, biomass growth, re-activation of dormant cells, and production of extracellular hydrolytic enzymes are possible. The latter, in turn, allows the microbial community to access more of the available external organic substrates. In the opposite case, active cells decay or become dormant. We apply the model to simulate the anaerobic degradation of cellulose by a hypothetical microbial community consisting of cellulolytic fermenting bacteria and sulfate-reducing bacteria, under conditions representative of those encountered in water-saturated subsurface environments.

Mollisols support the most productive agroecosystems in the world. Despite their critical links to food quality and human health, the varying distributions of selenium (Se) species and factors governing Se mobility in the mollisol vadose zone remain elusive. This research reveals that, in northern mollisol agroecosystems, Se hotspots (≥0.32 mg/kg) prevail along the regional river systems draining the Lesser Khingan Mountains, where piedmont Se-rich oil shales are the most probable source of regional Se. While selenate and selenite dominate Se species in the water-soluble and absorbed pools, mollisol organic matter is the major host for Se. Poorly crystalline and crystalline Fe oxides are subordinate in Se retention, hosting inorganic and organic Se at levels comparable to those in the adsorbed pool. The depth-dependent distributions of mollisol Se species for the non-cropland and cropland sites imply a predominance of reduced forms of Se under the mildly acidic and reducing conditions that, in turn, are variably impacted by agricultural land use. These findings therefore highlight that fluvial deposition and land use change together are the main drivers of the spatial variability and speciation of mollisol Se.

Lakes are key ecosystems within the global biogeosphere. However, the environmental controls on the biological productivity of lakes – including surface temperature, ice phenology, nutrient loads, and mixing regime – are increasingly altered by climate warming and land-use changes. To better characterize global trends in lake productivity, we assembled a dataset on chlorophyll-a concentrations as well as associated water quality parameters and surface solar radiation for temperate and cold-temperate lakes experiencing seasonal ice cover. We developed a method to identify periods of rapid net increase of in situ chlorophyll-a concentrations from time series data and applied it to data collected between 1964 and 2019 across 343 lakes located north of 40∘. The data show that the spring chlorophyll-a increase periods have been occurring earlier in the year, potentially extending the growing season and increasing the annual productivity of northern lakes. The dataset on chlorophyll-a increase rates and timing can be used to analyze trends and patterns in lake productivity across the northern hemisphere or at smaller, regional scales. We illustrate some trends extracted from the dataset and encourage other researchers to use the open dataset for their own research questions. The PCI dataset and additional data files can be openly accessed at the Federated Research Data Repository at https://doi.org/10.20383/102.0488 (Adams et al., 2021).

Previous work has shown that about 10% of total clay-bound Fe(III) in unaltered nontronite NAu-1 is bioreducible, although it remains unclear how much of the bioreducible Fe pool persists after repeated oscillations between anoxic and oxic conditions. Here, we report on results from an experiment where we monitored the abundance of bioreducible Fe(III) in NAu-1 over three consecutive redox cycles using chemical extractions and Fe isotope analysis to document the changes in the nature and extent of Fe atom exchange. During each cycle, NAu-1 was reduced biotically by Shewanella oneidensis MR-1 and then re-oxidized abiotically by O2 via aeration. By the third reduction period (RP3), the bacteria were only able to reduce 5.7% of the total clay Fe, that is, 40% less than during the first reduction period (RP1). The decrease in bioreducible Fe(III) is attributed to preferential reductive dissolution of Fe(III) from the finest clay particles. Extrapolation of the observed trend implies that, once the reducible Fe of the finest clay particles is removed, around 4% of the total Fe of the clay remains permanently redox-active, presumably as Fe atoms within the octahedral mineral structure that are accessible to the bacteria. The proposed particle size-dependent evolution of bioreducible Fe(III) from RP1 to RP3 is supported by the observed increasing crystalline domain size, preferential Fe dissolution from the smallest aggregates, and decreasing Fe isotope fractionation factors between aqueous Fe(II) and structural Fe(III) and between solid-bound Fe(II) and structural Fe(III). Our results imply that, in redox dynamic environments, the fraction of insoluble clay-bound Fe that is potentially renewable for use by Fe-reducing bacteria is a function of the evolving size distribution of the clay particles.

The availability of dissolved silicon (DSi) exerts an important control on phytoplankton communities in freshwater environments: DSi limitation can shift species dominance to non-siliceous algae and increase the likelihood of harmful algal blooms. The availability of DSi in the water column in turn depends on the dissolution kinetics of amorphous silica (ASi), including diatoms frustules and phytoliths. Here, batch dissolution experiments conducted with diatom frustules from three diatom species and synthetic Aerosil OX 50 confirmed the previously reported non-linear dependence of ASi dissolution rate on the degree of undersaturation of the aqueous solution. At least two first-order dissolution rate constants are therefore required to describe the dissolution kinetics at high (typically, ≥0.55) and low (typically,0.55) degrees of undersaturation. Our results further showed aqueous ferrous ion (Fe

The Three Gorges Reservoir (TGR), China, is the largest man-made reservoir in the world. Harmful algal blooms (HABs) have become common since the reservoir’s impoundment in 2003. To investi...

Flavin-mediated electron transfer is an important pathway for Fe(III) reduction by dissimilatory iron-reducing bacteria. Although the mechanisms and kinetics of Fe(III) reduction by reduced flavins have been widely studied, the reaction between Fe(II) and oxidized flavins is rarely investigated. Results of this study show that under anoxic conditions, Fe(II) can be oxidized by the oxidized forms of riboflavin (RBF) and flavin mononucleotide (FMN) at pH 7-9. For instance, at pH 9, 73% of 17.8 μM Fe(II) was oxidized by 10 μM RBF within 20 min. Both the rate and extent of oxidation increased with increasing concentrations of oxidized flavins and increasing solution pH. Thermodynamic calculations and kinetic analyses implied that the oxidation of Fe(II) proceeded predominantly via the autodecomposition of Fe2+-RBF- and Fe2+-FMN- complexes, along with minor contributions from direct oxidation of Fe(II) by flavins and flavin radicals. Our findings suggest that the reoxidation of Fe(II) by oxidized flavins may be a rate-controlling factor in microbial Fe(III) reduction via flavin-mediated electron transfer.

Although the majority of coastal sediments consist of sandy material, in some areas marine ingression caused the submergence of terrestrial carbon‐rich peat soils. This affects the coastal carbon balance, as peat represents a potential carbon source. We performed a column experiment to better understand the coupled flow and biogeochemical processes governing carbon transformations in submerged peat under coastal fresh groundwater (GW) discharge and brackish water intrusion. The columns contained naturally layered sediments with and without peat (organic carbon content in peat 39 ± 14 wt%), alternately supplied with oxygen‐rich brackish water from above and oxygen‐poor, low‐saline GW from below. The low‐saline GW discharge through the peat significantly increased the release and ascent of dissolved organic carbon (DOC) from the peat (δ13CDOC − 26.9‰ to − 27.7‰), which was accompanied by the production of dissolved inorganic carbon (DIC) and emission of carbon dioxide (CO2), implying DOC mineralization. Oxygen respiration, sulfate (urn:x-wiley:00243590:media:lno11438:lno11438-math-0001) reduction, and methane (CH4) formation were differently pronounced in the sediments and were accompanied with higher microbial abundances in peat compared to sand with urn:x-wiley:00243590:media:lno11438:lno11438-math-0002‐reducing bacteria clearly dominating methanogens. With decreasing salinity and urn:x-wiley:00243590:media:lno11438:lno11438-math-0003 concentrations, CH4 emission rates increased from 16.5 to 77.3 μmol m−2 d−1 during a 14‐day, low‐saline GW discharge phase. In contrast, oxygenated brackish water intrusion resulted in lower DOC and DIC pore water concentrations and significantly lower CH4 and CO2 emissions. Our study illustrates the strong dependence of carbon cycling in shallow coastal areas with submerged peat deposits on the flow and mixing dynamics within the subterranean estuary.

Lakes are key ecosystems within the global biogeosphere. However, the bottom-up controls on the biological productivity of lakes, including surface temperature, ice phenology, nutrient loads and mixing regime, are increasingly altered by climate warming and land-use changes. To better understand the environmental drivers of lake productivity, we assembled a dataset on chlorophyll-a concentrations, as well as associated water quality parameters and surface solar irradiance, for temperate and cold-temperate lakes experiencing seasonal ice cover. We developed a method to identify periods of rapid algal growth from in situ chlorophyll-a time series data and applied it to measurements performed between 1964 and 2019 across 357 lakes, predominantly located north of 40°. Long-term trends show that the algal growth windows have been occurring earlier in the year, thus potentially extending the growing season and increasing the annual productivity of northern lakes. The dataset is also used to analyze the relationship between chlorophyll-a growth rates and solar irradiance. Lakes of higher trophic status exhibit a higher sensitivity to solar radiation, especially at moderate irradiance values during spring. The lower sensitivity of chlorophyll-a growth rates to solar irradiance in oligotrophic lakes likely reflects the dominant role of nutrient limitation. Chlorophyll-a growth rates are significantly influenced by light availability in spring but not in summer and fall, consistent with a switch to top-down control of summer and fall algal communities. The growth window dataset can be used to analyze trends in lake productivity across the northern hemisphere or at smaller, regional scales. We present some general trends in the data and encourage other researchers to use the open dataset for their own research questions.

Peat accumulation in high latitude wetlands represents a natural long-term carbon sink, resulting from the cumulative excess of growing season net ecosystem production over non-growing season (NGS) net mineralization in soils. With high latitudes experiencing warming at a faster pace than the global average, especially during the NGS, a major concern is that enhanced mineralization of soil organic carbon will steadily increase CO2 emissions from northern peatlands. In this study, we conducted laboratory incubations with soils from boreal and temperate peatlands across Canada. Peat soils were pretreated for different soil moisture levels, and CO2 production rates were measured at 12 sequential temperatures, covering a range from − 10 to + 35 °C including one freeze–thaw event. On average, the CO2 production rates in the boreal peat samples increased more sharply with temperature than in the temperate peat samples. For same temperature, optimum soil moisture levels for CO2 production were higher in the peat samples from more flooded sites. However, standard reaction kinetics (e.g., Q10 temperature coefficient and Arrhenius equation) failed to account for the apparent lack of temperature dependence of CO2 production rates measured below 0 °C, and a sudden increase after a freezing event. Thus, we caution against using the simple kinetic expressions to represent the CO2 emissions from northern peatlands, especially regarding the long NGS period with multiple soil freeze and thaw events.

This report summarizes the group discussions and priorities on microplastics data management that emerged from a virtual workshop hosted by the University of Waterloo���s Water Institute, the Federated Research Data Repository (FRDR), and the Gordon Foundation., The workshop is funded by Compute Ontario. Additional support was provided by the NSERC/ECCC Alliance Grants - Plastics science for a cleaner future program, the Global Water Futures Program, University of Waterloo Library, Federated Research Data Repository and the Gordon Foundation

The interface between rivers and groundwater is a key driver for the turnover of reactive nitrogen compounds, that cause eutrophication of rivers and endanger drinking-water production from groundw...