Spatial and temporal variations in riverine mercury in the Mackenzie River Basin, Canada, from community-based water quality monitoring data.

Arctic rivers deliver ~40 t yr-1 of mercury (Hg) to the Arctic Ocean, ~6 % of which is from the Mackenzie River Basin (MRB), a region warming at ~3 times the mean hemispheric rate. How this will affect Hg transfer to ecosystems of the Beaufort Sea is a worrying issue. To help address this question, we analyzed >500 measurements of Hg and other water properties from 22 rivers collected in 2012-2018 by communities of the MRB. This new dataset provides a more comprehensive view of riverine Hg variations across the basin than was previously available. We find that rivers issued from mountains in the western MRB contribute the largest share of Hg in the Mackenzie River, 60-95 % of it being carried as fine suspended solids and probably sourced from riverbank erosion and thaw slumps. In contrast, lowland rivers of the central and eastern MRB contribute larger shares of dissolved Hg (up to 78 %), likely from recent atmospheric deposition through precipitation. Using load modelling constrained by the new water quality dataset, we estimate that the three largest western tributaries (Liard, Peel and Arctic Red rivers) of the Mackenzie contribute 60 % of the annual MRB THg export and DHg export to the Beaufort Sea during freshet, as well as 51 % of DHg export, while supplying 60 % of freshet discharge. Load modelling also reveals a sustained decline in DHg loads of ~13 kg yr-1 between 2001 and 2016 in the lower Mackenzie River, which likely reflect a decreasing trend in atmospheric Hg deposition over most of northwestern Canada during this period. This study highlights the value of community-based water quality monitoring in helping to support assessments of riverine Hg in the MRB in support of the Minamata Convention on Mercury.

Sources of riverine mercury across the Mackenzie River Basin; inferences from a combined HgC isotopes and optical properties approach.

The Arctic 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, δ202Hg), 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.

Multiple sources and sinks of dissolved inorganic carbon across Swedish streams, refocusing the lens of stable C isotopes.

It is well established that stream dissolved inorganic carbon (DIC) fluxes play a central role in the global C cycle, yet the sources of stream DIC remain to a large extent unresolved. Here, we explore large-scale patterns in δ13C-DIC from streams across Sweden to separate and further quantify the sources and sinks of stream DIC. We found that stream DIC is governed by a variety of sources and sinks including biogenic and geogenic sources, CO2 evasion, as well as in-stream processes. Although soil respiration was the main source of DIC across all streams, a geogenic DIC influence was identified in the northernmost region. All streams were affected by various degrees of atmospheric CO2 evasion, but residual variance in δ13C-DIC also indicated a significant influence of in-stream metabolism and anaerobic processes. Due to those multiple sources and sinks, we emphasize that simply quantifying aquatic DIC fluxes will not be sufficient to characterise their role in the global C cycle.

Aquatic export of young dissolved and gaseous carbon from a pristine boreal fen: Implications for peat carbon stock stability.

The stability of northern peatland's carbon (C) store under changing climate is of major concern for the global C cycle. The aquatic export of C from boreal peatlands is recognized as both a critical pathway for the remobilization of peat C stocks as well as a major component of the net ecosystem C balance (NECB). Here, we present a full year characterization of radiocarbon content (14 C) of dissolved organic carbon (DOC), carbon dioxide (CO2 ), and methane (CH4 ) exported from a boreal peatland catchment coupled with 14 C characterization of the catchment's peat profile of the same C species. The age of aquatic C in runoff varied little throughout the year and appeared to be sustained by recently fixed C from the atmosphere (<60 years), despite stream DOC, CO2 , and CH4 primarily being sourced from deep peat horizons (2-4 m) near the mire's outlet. In fact, the 14 C content of DOC, CO2 , and CH4 across the entire peat profile was considerably enriched with postbomb C compared with the solid peat material. Overall, our results demonstrate little to no mobilization of ancient C stocks from this boreal peatland and a relatively large resilience of the source of aquatic C export to forecasted hydroclimatic changes.

Patterns in CH4 and CO2 concentrations across boreal rivers: Major drivers and implications for fluvial greenhouse emissions under climate change scenarios.

It is now widely accepted that boreal rivers and streams are regionally significant sources of carbon dioxide (CO2), yet their role as methane (CH4) emitters, as well as the sensitivity of these greenhouse gas (GHG) emissions to climate change, are still largely undefined. In this study, we explore the large-scale patterns of fluvial CO2 and CH4 partial pressure (pCO2 , pCH4) and gas exchange (k) relative to a set of key, climate-sensitive river variables across 46 streams and rivers in two distinct boreal landscapes of Northern Québec. We use the resulting models to determine the direction and magnitude of C-gas emissions from these boreal fluvial networks under scenarios of climate change. River pCO2 and pCH4 were positively correlated, although the latter was two orders of magnitude more variable. We provide evidence that in-stream metabolism strongly influences the dynamics of surface water pCO2 and pCH4 , but whereas pCO2 is not influenced by temperature in the surveyed streams and rivers, pCH4 appears to be strongly temperature-dependent. The major predictors of ambient gas concentrations and exchange were water temperature, velocity, and DOC, and the resulting models indicate that total GHG emissions (C-CO2 equivalent) from the entire network may increase between by 13 to 68% under plausible scenarios of climate change over the next 50 years. These predicted increases in fluvial GHG emissions are mostly driven by a steep increase in the contribution of CH4 (from 36 to over 50% of total CO2 -equivalents). The current role of boreal fluvial networks as major landscape sources of C is thus likely to expand, mainly driven by large increases in fluvial CH4 emissions.