Dissolved Organic Carbon Trends Research Articles

Has lake brownification ceased? Stabilization, re-browning, and other factors associated with dissolved organic matter trends in eastern Canadian lakes

The increase in dissolved organic carbon (DOC) concentrations in freshwater systems has received considerable attention due to its implications for drinking water treatment and numerous limnological processes. While past studies have documented the influence of recovery from acidification and climate change on long-term DOC trends, the emerging importance of these explanatory factors remains less understood. In addition, few studies have followed up on recent trends in sites that have undergone increases in DOC. Using a dataset from 1980 to 2020, we investigated interannual variations in DOC and dissolved organic nitrogen (DON) in 49 lakes across four eastern Canadian regions with a history of increases in DOC. We identified recent shifts in DOC patterns using LOESS smoothing and piecewise regression. We observed a stabilizing pattern or even a decrease (p < 0.001) in high acidification regions (Dorset and Nova Scotia), where increases in DOC were previously documented. At the low acid deposition region, IISD-Experimental Lakes Area, an increasing pattern in DOC stabilized in the early 2000s; however, DOC appears to be increasing again in recent years (p = 0.03). Our analysis identified precipitation and SO4 deposition as the primary explanatory variables for DOC patterns (explaining 56–71% of variance). However, because acid deposition has declined substantially, climate and local watershed factors are becoming increasingly influential, leading to the emergence of new DOC patterns. Long-term changes in DOC and DON were not always synchronous, as these were often correlated with different factors (e.g., DON with ammonium deposition). This resulted in observable shifts in DOC:DON ratios, indicative of changes in dissolved organic matter (DOM) composition. We underscore the importance of ongoing monitoring in diverse regions because of the changing nature of environmental variables and new emerging trends.

Several Mechanisms Drive the Heterogeneity in Browning Across a Boreal Stream Network

AbstractOver the past few decades, many catchments in Northern hemisphere have experienced increases in dissolved organic carbon (DOC) concentrations, resulting in a brownish color of the water, known as aquatic browning. Several mechanisms have been proposed to explain browning, but consensus regarding the relative importance of recovery from acid deposition, climate change, and land management remains elusive. To advance our understanding of browning mechanisms, we explored DOC trends across 13 nested boreal catchments, leveraging concurrent hydrological, chemical, and terrestrial ecosystem data to quantify the contributions of different drivers on observed trends. We first identified the related environmental factors, then attributed the individual trends of DOC to potential drivers across space and time. Our results showed that all catchments exhibited increased DOC trends from 2003 to 2021, but the DOC response rates differed by five‐fold. No single mechanism could fully explain the browning; instead, sulfate deposition, climate‐related factors, and site properties jointly controlled the variation in DOC trends. Specifically, the long‐term increases in DOC were primarily driven by recovery from sulfate deposition, followed by increases in terrestrial productivity, temperature, and discharge. However, catchment area and landcover type also regulated the response rate of DOC to these drivers, creating spatial heterogeneity in browning among sub‐catchments despite similar deposition and climate forcing. Interestingly, browning has weakened in the last decade as sulfate deposition has fully recovered and other current drivers are insufficient to sustain the long‐term increases. Our results highlight that multifaceted, spatially structured, and nonstationary drivers must be accounted for to predict future DOC changes.

The role of dissolved organic carbon in Great Smoky Mountains National Park streams impacted by long-term acid deposition.

Following reductions in acid deposition in the Great Smoky Mountains National Park (GRSM) since the 2000s, many streams remain acidic and the role of organic acids (OA-) remains unknown due to limited OA- data. This study investigated dissolved organic carbon (DOC) concentrations as a surrogate for OA- across GRSM and its relationships with watershed characteristics, seasons, flow, and stream chemistry. Baseflow water samples were collected from seven watersheds for 2years and stormflow samples from three watersheds for 1year. During baseflow, DOC concentrations ranged from < 0.04 to 2.29mg L-1 with watershed medians between 0.61 and 1.00mg L-1. Stormflow DOC concentrations ranged from 1.36 to 5.66mg L-1. During the summer, median DOC concentrations were about twice that of the other three seasons. Stream DOC concentrations decreased with increasing elevation during baseflow but increased with increasing elevation during stormflow. Considering high elevations historically received greater acid deposition, this gradient between baseflow and stormflow suggests higher elevation streams are more impacted by OA-. Based on an OA-/DOC acidity model, it was estimated that during baseflow OA- was a minor contributor to stream acidity, in the order of 5.3 μeq L-1, however stormflow OA- was estimated at 52.5 μeq L-1, contributing to nearly half of stream acidity. Baseflow DOC was significantly correlated with pH and Ca2+, suggesting stream acidification/recovery is governed by base cations and Ca2+ availability. Furthermore, this study provides essential data for future research to evaluate stream DOC trends during acidification recovery and changes in biogeochemical processes.

Enhanced Role of Streamflow Processes in the Evolutionary Trends of Dissolved Organic Carbon.

Investigating dissolved organic carbon (DOC) dynamics and drivers in rivers enhances the understanding of carbon-environment linkages and support sustainability. Previous studies did not fully consider the dynamic nature of key drivers that influence the long-term changing trends in DOC concentration over time (the controlling factors and their roles in DOC trend can undergo alterations over time). We analyzed 42 years (1979-2018) of hydrometeorology, sulfate SO4, and DOC data from a 5.42 km2 watershed in central-southern Ontario, Canada. Our findings reveal a significant (p ≤ 0.01) overall increase in DOC concentrations, mainly due to the coevolution of SO4 and streamflow trends, especially the extreme flows. Over the 42-year period, the changing trend of streamflow (especially the extreme high or low flows) have significantly (p < 0.05) intensified their influence on DOC trends, increasing by an average of 30%. Conversely, the impact of SO4 has weakened, experiencing an average decrease of 32.6%. The upward trend in the annual average DOC concentration is attributed to the increasing number of maximum flow days within a year, while the decreasing trend in the number of minimum flow days has a contrasting effect. In other words, changes in maximum and minimum flow days have a counteracting effect on the DOC concentration trends. These results underscore the importance of considering the effects of altered streamflow processes on carbon cycle changes under evolving environmental conditions.

Recent, widespread nitrate decreases may be linked to persistent dissolved organic carbon increases in headwater streams recovering from past acidic deposition

Long-term monitoring of water quality responses to natural and anthropogenic perturbation of watersheds informs policies for managing natural resources. Dissolved organic carbon (DOC) and nitrate (NO3−) in streams draining forested landscapes provide valuable information on ecosystem function due to their biogeochemical reactivity and solubility in water. Here we evaluate a 20-year record (2001−2021) of biweekly stream-water samples (n > 3000) and continuous discharge in three forested catchments in the Adirondack region of New York to investigate and interpret long-term trends in DOC and NO3− concentrations. Results from the intensively monitored catchments were compared with data from synoptic surveys of streams throughout the Adirondack region. A weighted regressions on time, discharge, and season (WRTDS) model, used to estimate daily flow-normalized concentrations, determined that DOC increased by ~30 to 50 % while NO3− decreased by ~50 to 70 % over the study period. The large amount of data from catchments with different soil properties permitted us to assess the relative effects of hydrology, season, and land cover factors on temporal trends in DOC and NO3− concentrations. We found weak evidence of climatic forcing of long-term increases in DOC, and instead contend that declining ionic strength in precipitation linked to declining anthropogenic acid deposition is driving DOC trends in stream waters. Nitrate concentrations were more variable but clearly decreased in recent years possibly related to declining N deposition. The recent increase in DOC:NO3− in all catchments indicates a major shift in stream stoichiometry that reflects changes in ecosystem functioning that may have important biogeochemical implications for terrestrial as well as aquatic ecosystems.

Quantification of Discharge‐Specific Effects on Dissolved Organic Matter Export From Major Arctic Rivers From 1982 Through 2019

AbstractLong‐term increases in Arctic river discharge have been well documented, and observations in the six largest Arctic rivers show strong positive correlations between dissolved organic carbon (DOC) concentration, river discharge, and chromophoric dissolved organic matter (CDOM) content. Here, observations of DOC and CDOM collected from 2009 to 2019 by the Arctic Great Rivers Observatory were used to estimate chromophoric DOC (CDOC) concentrations in the Kolyma, Lena, Mackenzie, Ob', Yenisey, and Yukon Rivers. All rivers except the Mackenzie showed significant positive correlations between annual watershed runoff and the proportion of the DOC that is chromophoric. Historical estimates of DOC and CDOC export were calculated for 1982–2019 by extrapolating the DOC and CDOC concentration—discharge relationships from 2009 to 2019 as a hindcast modeled estimate. For the six rivers combined, modeled DOC and CDOC exports increased, but CDOC increased faster than total DOC. The Lena and Ob' Rivers showed significant increases in DOC export individually, with annual trends of 39.1 and 20.4 Gg C yr−1 respectively. November–April (winter) DOC and CDOC exports increased in all rivers but the Yenisey, with the hindcast winter Kolyma export increasing by more than 20% per decade. There were no significant trends in discharge or associated DOC and CDOC fluxes during the observational period from 2009 to 2019; only when hindcasted values driven by changes in river discharge were analyzed did trends in DOC and CDOC emerge. This demonstrates how shifting seasonal distributions and increases in discharge can drive changes in DOC and CDOC concentrations and exports independent of other environmental factors.

Long‐Term Trends in pCO2 in Lake Surface Water Following Rebrowning

AbstractOver the last 40 years, dissolved organic carbon (DOC) has been increasing in freshwater across many boreal regions. The extent to which these long‐term changes have affected lake CO2 dynamics is unclear. We have studied the temporal trends in DOC and pressure of CO2 (pCO2) over 40 years in 15 lakes in two regions of Ontario (Canada) subjected to browning and the abatement of SO2 deposition. Whereas from 1980 to 1999 there were no significant trends in pCO2 in any of the lakes, a significant increase was observed from 2000 to 2017. Although DOC concentrations increased during the same period, pCO2 and DOC were only weakly coupled, and we hypothesize the existence of DOC thresholds that determine this coupling. The recent increases in pCO2, linked to shifts in the C balance of lakes, may be contributing to the observed declines in lake pH, leading to a re‐acidification of lakes.

Non-conservative behavior of dissolved organic carbon in a Georgia salt marsh creek indicates summer outwelling

Salt marshes are highly productive ecosystems that efficiently accumulate carbon. However, it remains unclear how much carbon is exported from salt marshes (i.e., outwelled) through creeks as dissolved organic carbon (DOC). Addressing this uncertainty is critical for quantifying net carbon accumulation and determining the role marshes play in broader coastal carbon cycles. Consequently, this study sought to quantify net DOC fluxes through Groves Creek, the tidally-driven main creek channel of Groves Creek salt marsh on the Georgia coast (USA). To do this, near-continuous records of water flux, salt flux, and DOC flux were determined in Groves Creek's primary creek channel at 10-min resolution over 16 months. At our study site, we found that generally more water flowed onto the marsh through Groves Creek's primary creek channel during flood tide than left this route during ebb tide. The remaining unsampled water balance was assumed to leave the marsh via secondary marsh channels and over the marsh edge. Due to this limitation, the conservative nature of salt was utilized alongside flow and DOC to determine net DOC trends in Grove Creek's primary creek channel. Cumulative net DOC-salt relationships are linear for most of the study, indicating DOC largely behaved conservatively in the creek channel and wider marsh system. However, a period of non-conservative behavior in which the cumulative net DOC:salt ratio decreased indicated net DOC outwelling (4.1–30.1 g DOC m−2 y−1) during summer 2014. Results indicate DOC outwelling events, as observed here, may occur in pulses during highly productive summer months. Resolving these “hot” moments of DOC export at high-temporal resolution across larger salt marsh ecosystems is required to assess the true extent and quantitative significance of DOC outwelling to coastal carbon cycles and ecology.

Shifting stoichiometry: Long-term trends in stream-dissolved organic matter reveal altered C:N ratios due to history of atmospheric acid deposition.

Dissolved organic carbon (DOC) and nitrogen (DON) are important energy and nutrient sources for aquatic ecosystems. In many northern temperate, freshwater systems DOC has increased in the past 50 years. Less is known about how changes in DOC may vary across latitudes, and whether changes in DON track those of DOC. Here, we present long‐term DOC and DON data from 74 streams distributed across seven sites in biomes ranging from the tropics to northern boreal forests with varying histories of atmospheric acid deposition. For each stream, we examined the temporal trends of DOC and DON concentrations and DOC:DON molar ratios. While some sites displayed consistent positive or negative trends in stream DOC and DON concentrations, changes in direction or magnitude were inconsistent at regional or local scales. DON trends did not always track those of DOC, though DOC:DON ratios increased over time for ~30% of streams. Our results indicate that the dissolved organic matter (DOM) pool is experiencing fundamental changes due to the recovery from atmospheric acid deposition. Changes in DOC:DON stoichiometry point to a shifting energy‐nutrient balance in many aquatic ecosystems. Sustained changes in the character of DOM can have major implications for stream metabolism, biogeochemical processes, food webs, and drinking water quality (including disinfection by‐products). Understanding regional and global variation in DOC and DON concentrations is important for developing realistic models and watershed management protocols to effectively target mitigation efforts aimed at bringing DOM flux and nutrient enrichment under control.

Drivers of Dissolved Organic Carbon Mobilization From Forested Headwater Catchments: A Multi Scaled Approach

Understanding and predicting catchment responses to a regional disturbance is difficult because catchments are spatially heterogeneous systems that exhibit unique moderating characteristics. Changes in precipitation composition in the Northeastern U.S. is one prominent example, where reduction in wet and dry deposition is hypothesized to have caused increased dissolved organic carbon (DOC) export from many northern hemisphere forested catchments; however, findings from different locations contradict each other. Using shifts in acid deposition as a test case, we illustrate an iterative “process and pattern” approach to investigate the role of catchment characteristics in modulating the steam DOC response. We use a novel dataset that integrates regional and catchment-scale atmospheric deposition data, catchment characteristics and co-located stream Q and stream chemistry data. We use these data to investigate opportunities and limitations of a pattern-to-process approach where we explore regional patterns of reduced acid deposition, catchment characteristics and stream DOC response and specific soil processes at select locations. For pattern investigation, we quantify long-term trends of flow-adjusted DOC concentrations in stream water, along with wet deposition trends in sulfate, for USGS headwater catchments using Seasonal Kendall tests and then compare trend results to catchment attributes. Our investigation of climatic, topographic, and hydrologic catchment attributes vs. directionality of DOC trends suggests soil depth and catchment connectivity as possible modulating factors for DOC concentrations. This informed our process-to-pattern investigation, in which we experimentally simulated increased and decreased acid deposition on soil cores from catchments of contrasting long-term DOC response [Sleepers River Research Watershed (SRRW) for long-term increases in DOC and the Susquehanna Shale Hills Critical Zone Observatory (SSHCZO) for long-term decreases in DOC]. SRRW soils generally released more DOC than SSHCZO soils and losses into recovery solutions were higher. Scanning electron microscope imaging indicates a significant DOC contribution from destabilizing soil aggregates mostly from hydrologically disconnected landscape positions. Results from this work illustrate the value of an iterative process and pattern approach to understand catchment-scale response to regional disturbance and suggest opportunities for further investigations.

Natural and anthropogenic impacts on the DOC characteristics in the Yellow River continuum

The Yellow River is the second largest river in China. Carbon transport by the Yellow River has significant influence on riverine carbon cycles in Asia. During the wet season, the riverine carbon was mainly found in dissolved form, i.e., dissolved organic carbon (DOC), along the entire course of the river. The distinct spatial variations of DOC concentration were observed at different reaches of the mainstream (p < 0.01), while the highest mean DOC concentration was generally observed at midstream (4.13 ± 0.91 mg/L). Carbon stable isotope analysis δ13C and C: N ratio of DOC, evidenced the sources of DOC in headwater and upstream were primarily the terrestrial plants (94% and 61%), but it was changed to soil organic matter (SOM) in mid- and downstream (36% and 37%), and the contribution of sewage to DOC were also increased to 17% and 18%. In the whole mainstream of the Yellow River, water temperature (WT) had a significant impact on DOC concentration, and it could explain 67% of the DOC variance. However, in a large catchment, the driving mechanisms on the DOC variations in headwaters will not necessarily be those controlling DOC trends in downstream. The study firstly quantified, in headwater and upstream, the natural factors explained as much as 65% and 73% of the DOC variations, respectively. In mid- and downstream areas, DOC was significantly influenced by the amount of wastewater discharged by the industry and the use of chemical fertilizers (p < 0.05). These findings may facilitate a better assessment of global riverine carbon cycling and may help to reveal the importance of the balance between development and environmental sustainability with the changing DOC transport features in the Yellow River due to human disturbances.

Inconsistent browning of northeastern U.S. lakes despite increased precipitation and recovery from acidification

AbstractMultiple studies have reported widespread browning of Northern Hemisphere lakes. Most examples are from boreal lakes that have experienced limited human influence, and browning has alternatively been attributed to changes in atmospheric deposition, climate, and land use. To determine the extent and possible causes of browning across a more geographically diverse region, we examined watercolor and dissolved organic carbon (DOC) time series in hundreds of northeastern U.S. lakes. The majority of lakes have increased in both DOC and color, but there were neither coherent spatial patterns in trends nor relationships with previously reported drivers. Color trends were more variable than DOC trends, and DOC and color trends were not strongly correlated, indicating a cause other than or in addition to increased loading of terrestrial carbon. Browning may be pronounced in regions where climate and atmospheric deposition are dominant drivers but muted in more human‐dominated landscapes with a limited extent of organic soils where other disturbances predominate.

Leaching of dissolved organic carbon from mineral soils plays a significant role in the terrestrial carbon balance.

The leaching of dissolved organic carbon (DOC) from soils to the river network is an overlooked component of the terrestrial soil C budget. Measurements of DOC concentrations in soil, runoff and drainage are scarce and their spatial distribution highly skewed towards industrialized countries. The contribution of terrestrial DOC leaching to the global‐scale C balance of terrestrial ecosystems thus remains poorly constrained. Here, using a process based, integrative, modelling approach to upscale from existing observations, we estimate a global terrestrial DOC leaching flux of 0.28 ± 0.07 Gt C year−1 which is conservative, as it only includes the contribution of mineral soils. Our results suggest that globally about 15% of the terrestrial Net Ecosystem Productivity (NEP, calculated as the difference between Net Primary Production and soil respiration) is exported to aquatic systems as leached DOC. In the tropical rainforest, the leached fraction of terrestrial NEP even reaches 22%. Furthermore, we simulated spatial‐temporal trends in DOC leaching from soil to the river networks from 1860 to 2010. We estimated a global increase in terrestrial DOC inputs to river network of 35 Tg C year−1 (14%) from 1860 to 2010. Despite their low global contribution to the DOC leaching flux, boreal regions have the highest relative increase (28%) while tropics have the lowest relative increase (9%) over the historical period (1860s compared to 2000s). The results from our observationally constrained model approach demonstrate that DOC leaching is a significant flux in the terrestrial C budget at regional and global scales.

Impacts of Droughts and Acidic Deposition on Long-Term Surface Water Dissolved Organic Carbon Concentrations in Upland Catchments in Wales

Concerns have been raised about rising trends in surface water dissolved organic carbon (DOC) concentrations in UK upland catchments over the past decades. Several mechanisms have been proposed to explain these trends, including changes in climate and declines in sulphate deposition across Europe. Drier summers and wetter winters are projected in the UK, and there is an increasing interest in whether the rising trends of DOC would be continued or stabilised. In this paper, the INCA (INtegrated CAtchment) water quality model was applied to the upland catchment of the River Severn at Plynlimon in Wales and used to simulate the effects of both climate and sulphate deposition on surface water DOC concentrations. We introduced new parameter sets of INCA to explain enzymatic latch effect in peatlands during droughts. The model was able to simulate recent past (1995-2013) rising trends in DOC in Plynlimon. Climatic projections were employed to estimate the future trends on DOC in the uplands and to consider potential impacts on catchment management. The model was run with climatic scenarios generated using the weather@home2 climate modelling platform and with sulphate deposition scenarios from the European Monitoring and Evaluation Programme (EMEP) for 1975-2100. The modelling results show that the rising DOC trends are likely to continue in the near future (2020-2049) and the level of DOC concentrations is projected to stabilise in the far future (2070-2099). However, in the far future, the seasonal patterns of DOC concentrations will change, with a post-drought DOC surge in autumn months.

Patterns and trends in lake concentrations of dissolved organic carbon in a landscape recovering from environmental degradation and widespread acidification

Concentrations of dissolved organic carbon (DOC) have increased in lakes throughout North America and Europe over the last three decades. Recovery from acid deposition and climate change have both been postulated as the primary mechanisms for the increase in DOC. To provide a clearer insight into the mechanisms responsible for increasing DOC we evaluated changes in lake and peat porewater chemistry collected in an area of approximately 33,000 km2 surrounding Sudbury, Ontario, a region undergoing dramatic recovery from acidic deposition. DOC concentrations varied considerably among the 44 lakes and over time (samples annually from 1981 to 2018), but the Sens Slope value showed a strong increase in lake DOC concentration over time, at 0.05 mg/ L y−1 (p < 0.001) that was related to increasing pH [0.03 units y−1, p < 0.001] and decreasing lake SO4 concentration [−0.24 mg/ L y−1; p < 0.001], but showed no relationship with temperature or precipitation. Similar strong relationships between DOC and pH (positive) and SO4 (negative) were observed in 18 peatlands sampled in the region. In a spatial analysis of 82 lakes sampled in 2018, concentrations of DOC in lakes were highest in flatter catchments with a greater wetland area, suggesting that wetlands are a major source of DOC in lakes. Optical properties of DOC obtained from extracts of wetland and upland soils at 6 catchments could be distinguished, primarily due to upland litter extracts having distinct optical properties from mineral soils or wetland soils. Optical properties of DOC in lakes however were inconsistent with those measured in soil extracts indicating that they are not useful for distinguishing DOC sources in these lakes. A predictive model was developed to explain DOC trends within Sudbury lakes using a stepwise linear regression combined with hierarchical partitioning to confirm the most influential processes on DOC. Almost 50% of the variability in DOC change in the 44 lakes was explained by the magnitude in lake pH change, catchment size and catchment sparse tree cover showing that recovery from acidic deposition is overwhelmingly responsible for increasing DOC in Sudbury lakes.

Climate, snowmelt dynamics and atmospheric deposition interact to control dissolved organic carbon export from a northern forest stream over 26 years

Increasing concentrations of dissolved organic carbon (DOC) have been identified in many freshwater systems over the last three decades. Studies have generally nominated atmospheric deposition as the key driver of this trend, with changes in climatic factors also contributing. However, there is still much uncertainty concerning net effects of these drivers on DOC concentrations and export dynamics. Changes in climate and climate mediated snowfall dynamics in northern latitudes have not been widely considered as causal factors of changes in long-term DOC trends, despite their disproportionate role in annual DOC export. We leveraged long-term datasets (1988–2013) from a first-order forested tributary of Lake Superior to understand causal factors of changes in DOC concentrations and exports from the watershed, by simultaneously evaluating atmospheric deposition, temperature, snowmelt timing, and runoff. We observed increases in DOC concentrations of approximately 0.14 mg C l−1 yr−1 (mean = 8.12 mg C l−1) that were related with declines in sulfate deposition (0.03 mg l−1 yr−1). Path analysis revealed that DOC exports were driven by runoff related to snowmelt, with peak snow water equivalences generally being lower and less variable in the 21st century, compared with the 1980s and 1990s. Mean temperatures were negatively related (direct effects) to maximum snow water equivalences (−0.71), and in turn had negative effects on DOC concentrations (−0.58), the timing of maximum discharge (−0.89) and DOC exports (indirect effect, −0.41). Based on these trends, any future changes in climate that lessen the dominance of snowmelt on annual runoff dynamics—including an earlier peak discharge—would decrease annual DOC export in snowmelt dominated systems. Together, these findings further illustrate complex interactions between climate and atmospheric deposition in carbon cycle processes, and highlight the importance of long-term monitoring efforts for understanding the consequences of a changing climate.

Re-browning of Sudbury (Ontario, Canada) lakes now approaches pre-acid deposition lake-water dissolved organic carbon levels

Since the implementation of large-scale lake monitoring in the ~1980s, water color and dissolved organic carbon (DOC) concentrations have increased in many northern lakes (i.e., lake browning), impacting the functioning of aquatic ecosystems. In regions that formerly experienced high levels of acid deposition, this browning trend has been largely attributed to the recovery from the impacts of past acid deposition. However, the extent to which DOC levels have now returned to naturally higher, pre-industrial conditions is still poorly understood. In this study, we assessed whether DOC levels are still influenced by acid deposition in lakes near Sudbury, Ontario, a region that has been heavily affected by sulfur dioxide emissions from local metal smelting during the 20th century. We analyzed water chemistry monitoring data (1981–2018), together with comparisons between modern and pre-industrial DOC levels inferred from sediment spectroscopy, for 51 acid-sensitive and 24 buffered reference lakes across the Sudbury landscape. Since 1981, DOC concentrations doubled in acid-sensitive lakes, with a mean increase of +1.6 mg/L, whereas in more buffered reference lakes, mean DOC levels increased by only 0.8 mg/L. Similarly, sediment-inferred DOC trends indicate that current DOC levels are, on average, ~22% below pre-industrial levels in acid sensitive systems compared to only ~10% in buffered lakes. Weakening correlations between DOC and acidification-related water chemistry variables (e.g., pH, alkalinity, metals) further indicate a diminishing influence of acid deposition on DOC in Sudbury lakes. These results highlight the strong impact that acid deposition has historically had on lake-water DOC dynamics in this region, but also suggest that DOC levels are approaching natural baseline levels in less acid-sensitive lakes, and that other drivers, such as changes in climate or vegetation cover, are now becoming the dominant controls on changes in DOC concentrations.

Effects of acidity on dissolved organic carbon in organic soil extracts, pore water and surface litters

Over the past 30–40 years, dissolved organic carbon (DOC) concentrations have increased in soil solutions and surface waters in many acid-sensitive areas of Europe and North America. This has been linked to recovery from acidification in response to decreasing levels of atmospheric pollution. Evidence from radiocarbon dating suggests that DOC in surface waters is typically derived from recently photosynthesised organic matter such as plant litter and exudates, yet there is little information on the pH-sensitivity of organic matter solubility, or its decomposition, in litter layers and in different organic soils. Therefore the purpose of this study was to determine a) the sensitivity of DOC to acidity in different surface layers and soil types, in order to b) improve understanding of the key sources contributing to the increasing DOC trend. Such information is vital for understanding site specific characteristics contributing to inconsistencies in DOC release between catchments, and for improving predictions of carbon fluxes and budgets.Based on data collected at four established field pH-manipulation experiments in upland areas of the United Kingdom, we examined the sources, composition and acid-sensitivity of DOC export from the litter and organic soils. We found that litter generated nearly three times more DOC than the organic soils, consistent with radiocarbon evidence that recent plant inputs are a major source of DOC. Furthermore, litter derived DOC had lower specific ultraviolet light absorbance (SUVA) than organic soil DOC, suggesting greater biodegradability, and was not acid sensitive. In contrast, organic soil DOC concentrations were more strongly related to experimentally manipulated pH, implying that the mobility of this DOC may be subject to physicochemical rather than biotic controls. Our results suggest that physicochemically mediated controls on organic matter solubility may be a key driver behind the widely observed increases in surface water DOC in areas undergoing recovery from acidification.

Predicted Impact of Climate Change on Trihalomethanes Formation in Drinking Water Treatment

Quantitative predictions of impacts on public water supplies are essential for planning climate change adaptations. Monitoring data from five full-scale Scottish drinking water treatment plants (DWTPs) showed that significant correlations exist between conditionally carcinogenic trihalomethanes (THMs) levels, water temperature (r = 0.812, p = 0.0013) and dissolved organic carbon (DOC) (r = 0.892, p < 0.0001), respectively. The strong seasonality of these parameters demonstrated how climate can influence THMs formation. We quantified with laboratory experiments the sensitivity of THMs formation to changes in water temperature and DOC concentration. The laboratory data accurately reproduced real-world THM formation in the DWTPs. We then combined these validated relationships with information from the literature about future trends in mean summer temperatures and surface water DOC in the British Isles, to estimate future global warming impacts on THMs formation in DWTPs that use chlorine for disinfection. An increase in mean summer temperatures will likely increase THM formation, with a 1.8 °C temperature increase and 39% THMs increase by 2050 representing our mid-range scenario. Such an increase has major implications to potable water around the world, either an increased health risk or increased water treatment costs to maintain an equivalent quality potable supply.

Multi-decadal trends and influences on dissolved organic carbon distribution in the Barataria Basin, Louisiana from in-situ and Landsat/MODIS observations

Barataria Basin, a deltaic marsh-estuary system in the northern Gulf of Mexico (nGOM), is an important source of dissolved organic matter (DOM) to the coastal ecosystem. To assess DOM dynamics, monthly measurements of dissolved organic carbon (DOC) concentrations and colored DOM (CDOM; an optical proxy for DOC) absorption were obtained over a three-year period (2008–2011) along a transect encompassing the upper, middle and lower regions of the Barataria Basin estuary. While CDOM absorption coefficient at 355 nm (ag355) generally decreased and spectral slope at 275–295 nm (S275–295) increased along the transect from the upper to lower basin, deviations were observed associated with hydrologic and meteorological influences. An application of wavelet analysis to the time-series of ag355 and various freshwater sources revealed a spatiotemporal resonance of ag355 with freshwater input from the Mississippi River (MR), the controlled freshwater discharge from the Davis Pond freshwater diversion, and rainfall in the lower, middle and upper basins, respectively. Field measurements and Landsat/MODIS data spanning across different seasons between 2008 and 2011 were used to develop optimized ag355 empirical algorithms for the high river flow, cold front, and normal conditions. Power law models relating a band ratio (green/red) of a satellite sensor to ag355 showed good performance for the MODIS-Aqua (R2~0.81–0.83, N = 581) and Landsat-5 TM (R2~0.72–0.79, N = 304) imagery. ag355-DOC relationships (R2~0.77–0.84, N = 306) applied to historical Landsat-5 TM (1985–2011) and MODIS-Aqua imagery (2002−2012) showed strong environmental influences on multi-decadal CDOM and DOC spatiotemporal trends. Satellite-derived DOC agreed reasonably well with in-situ measured DOC (averaged R2 = 0.71; RMSE = 2.13). While the time-series DOC showed seasonality and decreasing gradients from the upper to lower basin, an overall increase in DOC was observed in the upper and middle basins from 1985 to 2012. However, in the lower basin, DOC increased from 1985 to 2006 but decreased from 2007 to 2012, likely due to the impact of two major hurricanes in 2005. Furthermore, relationships between satellite-derived DOC and land cover variations (1985–2011) along the wetland-estuary interfaces derived from Landsat-5 TM supervised classification showed an increase in DOC with corresponding increase in developed area in the upper basin, while in the lower basin, DOC increased by 41% (R2 = 0.54) between 1985 and 2006 corresponding to a 17% decrease in salt marsh area, suggesting strong land use/land loss impact on the long-term DOC trends in Barataria Basin.