Riverine exports of organic and inorganic carbon (OC, IC) to oceans are intricately linked to processes occurring on land. Across high latitudes, thawing permafrost, alteration of hydrologic flow ...paths, and changes in vegetation may all affect this flux, with subsequent implications for regional and global carbon (C) budgets. Using a unique, multi-decadal dataset of continuous discharge coupled with water chemistry measurements for the Mackenzie River, we show major increases in dissolved OC (DOC) and IC (as alkalinity) fluxes since the early 1970s, for a watershed that covers 1.8 M km2 of northwestern Canada, and provides substantial inputs of freshwater and biogeochemical constituents to the Arctic Ocean. Over a 39-year period of record, DOC flux at the Mackenzie mouth increased by 39.3% (44.5 22.6 Gmol), while alkalinity flux increased by 12.5% (61.5 60.1 Gmol). Isotopic analyses and substantial increases in sulfate flux indicate that increases in alkalinity are driven by accelerating sulfide oxidation, a process that liberates IC from rock and soils in the absence of CO2 consumption. Seasonal and sub-catchment trends suggest that permafrost thaw plays an important role in the observed increases in DOC and alkalinity: sub-catchment increases for all constituents are confined to northern, permafrost-affected regions, while observed increases in autumn to winter are consistent with documented landscape-scale changes that have resulted from changing thaw dynamics. This increase in DOC and sulfide-derived alkalinity represents a substantial intensification of land-to-ocean C mobilization, at a level that is significant within the regional C budget. The change we observe, for example, is similar to current and projected future rates of CO2 consumption by weathering in the Mackenzie basin.
Uranium (U) isotope signatures (δ238U) recorded in sedimentary archives provide insight into the paleo redox state of the ocean. But the robust interpretation of these sedimentary U isotope records ...requires characterisation of the U isotope signature of rivers, the main source of U to the ocean. The main controlling factors on riverine δ238U remain poorly constrained. Here, we investigate the elemental and isotope signatures of uranium in the dissolved and solid loads of a well-characterised river, the Mackenzie Basin (Canada).
In the Mackenzie Basin, the solid load δ238U shows a positive relationship with U and vanadium (V) contents, consistent with the suggestion that particulate δ238U are explained by variable contributions via erosion of silicate and black shale. The δ238U of the dissolved and solid loads are correlated which, at first sight, suggests no U isotope fractionation during chemical weathering, and a purely lithological control on both the river dissolved and solid δ238U. Moreover, relationships between dissolved U and δ238U and major elements such as calcium and sulfate, also support the idea of a lithological control. However, the δ238U of end members inferred from mixing relationships are not consistent with binary mixing of two sources, suggesting some potential U isotope fractionation during weathering. In fact, the abundance of U in the river dissolved load is always lower than that predicted by silicate rock weathering. This suggests that 1) the weathering of silicate only can explain the abundance of U in the river dissolved load and 2) secondary weathering processes scavenge a proportion of the U released by primary mineral breakdown. The broad negative relationship between δ238U and the depletion of dissolved U is also consistent with the control of dissolved δ238U by secondary weathering processes following silicate mineral breakdown. The relationships observed between dissolved U, δ238U and the large-scale environmental controls on weathering processes (such as weathering intensity or runoff) support this hypothesis.
Overall, our interpretations of the variation in the river dissolved δ238U challenge the common assumption of the control of dissolved U by black shale and carbonate weathering. In addition, we suggest that the extent of secondary weathering processes can imprint on the U isotope signature of rivers, now and in the past.
Permafrost thaw in Arctic watersheds threatens to mobilize hitherto sequestered carbon. We examine the radiocarbon activity (F14C) of dissolved organic carbon (DOC) in the northern Mackenzie River ...basin. From 2003–2017, DOC‐F14C signatures (1.00 ± 0.04; n = 39) tracked atmospheric 14CO2, indicating export of “modern” carbon. This trend was interrupted in June 2018 by the widespread release of aged DOC (0.85 ± 0.16, n = 28) measured across three separate catchment areas. Increased nitrate concentrations in June 2018 lead us to attribute this pulse of 14C‐depleted DOC to mobilization of previously frozen soil organic matter. We propose export through lateral perennial thaw zones that occurred at the base of the active layer weakened by preceding warm summer and winter seasons. Although we are not yet able to ascertain the broader significance of this “anomalous” mobilization event, it highlights the potential for rapid and large‐scale release of aged carbon from permafrost.
Plain Language Summary
The thaw of continuously frozen grounds in the Arctic induced by regional warming accelerates the release of carbon to the atmosphere and river systems. Of particular concern is the fate of dissolved organic carbon (DOC) due to its potential for rapid oxidation to carbon dioxide. In order to understand the ramifications of a warming climate, we analyze the radiocarbon age of DOC in the northern Mackenzie River—a major Arctic river basin. DOC in large Arctic rivers has been characterized by young radiocarbon ages, from modern vegetation and surface soils. In June 2018, we recorded a departure from long‐term observations: Older DOC was measured in three large catchments draining into the Mackenzie Delta. This release of aged DOC followed a warm summer and the second warmest winter on record. We infer that the aged DOC derived from thaw of deeper soil horizons and subsequent carbon mobilization and riverine export. This is the first time such an event has been documented; it highlights the potential for abrupt and widespread aged DOC export with important implications for regional and global carbon cycles.
Key Points
A widespread pulse of aged dissolved organic carbon (DOC) occurred in the Mackenzie River and its tributaries in June 2018
Export of aged DOC is consistent with a prolonged warming period and the formation of supra‐permafrost taliks
Mobilization of aged DOC and nitrate suggests percolation of supra‐permafrost groundwater through previously frozen soil layers
Hydrological processes within the alpine tundra of the Taiga Cordillera ecozone in northwestern Canada are poorly understood, yet these areas receive more precipitation per unit area than lowlands ...and sustain late summer and winter flow in large river systems when contributions from other areas are reduced. The objective of this study was to quantify the spatial and temporal variability in streamflow and groundwater recharge within an alpine tundra basin with discontinuous permafrost and explore the potential impacts of climate change on the timing and intensity of these hydrological processes. Hydrometric and remote sensing methods were used to complete a water balance assessment of the study basin and compare spatial and seasonal differences in inputs, outputs, runoff ratio, and runoff–recharge partitioning during the 2019 open water season. During the freshet, the basin received large daily melt volumes and responded with highly efficient runoff. Evapotranspiration became the primary means of water loss in the early summer but declined as the summer progressed. During the summer, groundwater discharge exceeded precipitation inputs and sustained headwater subbasin streamflow. Groundwater recharge occurred primarily via glaciofluvial upland infiltration during the freshet and channel bed infiltration during the summer. The partitioning of basin outputs between runoff and groundwater recharge was highly seasonal, with a freshet ratio favoring runoff (0.83) while the early and late summer favored recharge (0.28 and 0.17, respectively). As climate change continues, higher air temperatures and greater precipitation are expected for the study basin. Longer open water seasons and declining permafrost extent within the study basin will result in a greater proportion of input water routed to storage and/or groundwater recharge instead of runoff. Shrubification and treeline expansion may also increase evaporative losses from alpine tundra areas, reducing both rapid runoff and delayed aquifer recharge contributions important for larger rivers at lower elevation.
The biomarker composition of dissolved organic carbon (DOC) of the six largest Arctic rivers was studied between 2003 and 2007 as part of the PARTNERS Project. Samples were collected over seasonal ...cycles relatively close to the river mouths. Here we report the lignin phenol and p-hydroxybenzene composition of Arctic river DOC in order to identify major sources of carbon. Arctic river DOC represents an important carbon conduit linking the large pools of organic carbon in the Arctic/Subarctic watersheds to the Arctic Ocean. Most of the annual lignin discharge (>75%) occurs during the two month of spring freshet with extremely high lignin concentrations and a lignin phenol composition indicative of fresh vegetation from boreal forests. The three large Siberian rivers, Lena, Yenisei, and Ob, which also have the highest proportion of forests within their watersheds, contribute about 90% of the total lignin discharge to the Arctic Ocean. The composition of river DOC is also characterized by elevated levels of p-hydroxybenzenes, particularly during the low flow season, which indicates a larger contribution from mosses and peat bogs. The lignin composition was strongly related to the average 14C-age of DOC supporting the abundance of young, boreal-vegetation-derived leachates during spring flood, and older, soil-, peat-, and wetland-derived DOC during groundwater dominated low flow conditions, particularly in the Ob and Yukon Rivers. We observed significant differences in DOC concentration and composition between the rivers over the seasonal cycles with the Mackenzie River being the most unique, the Lena River being similar to the Yenisei, and the Yukon being most similar to the Ob. The observed relationship between the lignin phenol composition and watershed characteristics suggests that DOC discharge from these rivers could increase in a warmer climate under otherwise undisturbed conditions.
The erosion of major mountain ranges is thought to be largely cannibalistic, recycling sediments that were deposited in the ocean or on the continents prior to mountain uplift. Despite this ...recognition, it has not yet been possible to quantify the amount of recycled material that is presently transported by rivers to the ocean. Here, we have analyzed the Li content and isotope composition (δLi7) of suspended sediments sampled along river depth profiles and bed sands in three of the largest Earth's river systems (Amazon, Mackenzie and Ganga–Brahmaputra rivers). The δLi7 values of river-sediments transported by these rivers range from +5.3 to −3.6‰ and decrease with sediment grain size. We interpret these variations as reflecting a mixture of unweathered rock fragments (preferentially transported at depth in the coarse fraction) and present-day weathering products (preferentially transported at the surface in the finest fraction). Only the finest surface sediments contain the complementary reservoir of Li solubilized by water–rock interactions within the watersheds. Li isotopes also show that river bed sands can be interpreted as a mixture between unweathered fragments of igneous and sedimentary rocks. A mass budget approach, based on Li isotopes, Li/Al and Na/Al ratios, solved by an inverse method allows us to estimate that, for the large rivers analyzed here, the part of solid weathering products formed by present-day weathering reactions and transported to the ocean do not exceed 35%. Li isotopes also show that the sediments transported by the Amazon, Mackenzie and Ganga–Brahmaputra river systems are mostly sourced from sedimentary rocks (>60%) rather than igneous rocks. This study shows that Li isotopes in the river particulate load are a good proxy for quantifying both the erosional rock sources and the fingerprint of present-day weathering processes. Overall, Li isotopes in river sediments confirm the cannibalistic nature of erosion and weathering.
•We measured δLi7 in Amazon, Mackenzie and Ganga–Brahmaputra sediment depth-profiles.•The δLi7 of river sediments is related to sediment grain size.•River sediments δLi7 record both provenance and present-day weathering.•More than 60% river sediments are sourced from sedimentary rocks.•Less than 35% river sediments are formed by present-day weathering.
The Arctic terrestrial environment harbors a complex mosaic of mercury (Hg) and carbon (C) reservoirs, some of which are rapidly destabilizing in response to climate warming. The sources of riverine ...Hg across the Mackenzie River basin (MRB) are uncertain, which leads to a poor understanding of potential future release. Measurements of dissolved and particulate mercury (DHg, PHg) and carbon (DOC, POC) concentration were performed, along with analyses of Hg stable isotope ratios (incl. ∆199Hg, d202Hg), radiocarbon content (∆14C) and optical properties of DOC of river water. Isotopic ratios of Hg revealed a closer association to terrestrial Hg reservoirs for the particulate fraction, while the dissolved fraction was more closely associated with atmospheric deposition sources of shorter turnover time. There was a positive correlation between the ∆14C-OC and riverine Hg concentration for both particulate and dissolved fractions, indicating that waters transporting older-OC (14C-depleted) also contained higher levels of Hg. In the dissolved fraction, older DOC was also associated with higher molecular weight, aromaticity and humic content, which are likely associated with higher Hg-binding potential. Riverine PHg concentration increased with turbidity and SO4 concentration. There were large contrasts in Hg concentration and OC age and quality among the mountain and lowland sectors of the MRB, which likely reflect the spatial distribution of various terrestrial Hg and OC reservoirs, including weathering of sulfate minerals, erosion and extraction of coal deposits, thawing permafrost, forest fires, peatlands, and forests. Results revealed major differences in the sources of particulate and dissolved riverine Hg, but nonetheless a common positive association with older riverine OC. These findings reveal that a complex mixture of Hg sources, supplied across the MRB, will contribute to future trends in Hg export to the Arctic Ocean under rapid environmental changes.
Much of the world's boreal forest occurs on permafrost (perennially cryotic ground). As such, changes in permafrost conditions have implications for forest function and, within the zone of ...discontinuous permafrost (30–80% permafrost in areal extent), distribution. Here, forested peat plateaus underlain by permafrost are elevated above the surrounding permafrost‐free wetlands; as permafrost thaws, ground surface subsidence leads to waterlogging at forest margins. Within the North American subarctic, recent warming has produced rapid, widespread permafrost thaw and corresponding forest loss. Although permafrost thaw‐induced forest loss provides a natural analogue to deforestation occurring in more southerly locations, we know little about how fragmentation relates to subsequent permafrost thaw and forest loss or the role of changing conditions at the edges of forested plateaus. We address these knowledge gaps by (i) examining the relationship of forest loss to the degree of fragmentation in a boreal peatland in the Northwest Territories, Canada; and (ii) quantifying associated biotic and abiotic changes occurring across forest‐wetland transitions and extending into the forested plateaus (i.e., edge effects). We demonstrate that the rate of forest loss correlates positively with the degree of fragmentation as quantified by perimeter to area ratio of peat plateaus (edge : area). Changes in depth of seasonal thaw, soil moisture, and effective leaf area index (LAIₑ) penetrated the plateau forests by 3–15 m. Water uptake by trees was sevenfold greater in the plateau interior than at the edges with direct implications for tree radial growth. A negative relationship existed between LAIₑ and soil moisture, suggesting that changes in vegetation physiological function may contribute to changing edge conditions while simultaneously being affected by these changes. Enhancing our understanding of mechanisms contributing to differential rates of permafrost thaw and associated forest loss is critical for predicting future interactions between the land surface processes and the climate system in high‐latitude regions.
Canada’s Mackenzie River Basin (MRB) is one of the largest relatively pristine ecosystems in North America. Home to indigenous peoples for millennia, the basin is also the site of increasing resource ...development, notably fossil fuels, hydroelectric power resources, minerals, and forests. Three provinces, three territories, the Canadian federal government, and Aboriginal governments (under Canada’s constitution, indigenous peoples are referred to as “Aboriginal”) have responsibilities for water in the basin, making the MRB a significant setting for cooperative, transboundary water governance. A framework agreement that provides broad principles and establishes a river basin organization, the MRB Board, has been in place since 1997. However, significant progress on completing bilateral agreements under the 1997 Mackenzie River Basin Transboundary Waters Master Agreement has only occurred since 2010. We considered the performance of the MRB Board relative to its coordination function, accountability, legitimacy, and overall environmental effectiveness. This allowed us to address the extent to which governance based on river basin boundaries, a bioregional approach, could contribute to adaptive governance in the MRB. Insights were based on analysis of key documents and published studies, 19 key informant interviews, and additional interactions with parties involved in basin governance. We found that the MRB Board’s composition, its lack of funding and staffing, and the unwillingness of the governments to empower it to play the role envisioned in the Master Agreement mean that as constituted, the board faces challenges in implementing a basin-wide vision. This appears to be by design. The MRB governments have instead used the bilateral agreements under the Master Agreement as the primary mechanism through which transboundary governance will occur. A commitment to coordinating across the bilateral agreements is needed to enhance the prospects for adaptive governance in the basin.
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