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Soils of the northern high latitudes store carbon over millennial timescales (thousands of years) and contain approximately double the carbon stock of the atmosphere. Warming and associated permafrost thaw can expose soil organic carbon and result in mineralization and carbon dioxide (CO2) release. However, some of this soil organic carbon may be eroded and transferred to rivers. If it escapes degradation during river transport and is buried in marine sediments, then it can contribute to a longer-term (more than ten thousand years), geological CO2 sink. Despite this recognition, the erosional flux and fate of particulate organic carbon (POC) in large rivers at high latitudes remains poorly constrained. Here, we quantify the source of POC in the Mackenzie River, the main sediment supplier to the Arctic Ocean, and assess its flux and fate. We combine measurements of radiocarbon, stable carbon isotopes and element ratios to correct for rock-derived POC. Our samples reveal that the eroded biospheric POC has resided in the basin for millennia, with a mean radiocarbon age of 5,800 ± 800 years, much older than the POC in large tropical rivers. From the measured biospheric POC content and variability in annual sediment yield, we calculate a biospheric POC flux of 2.2(+1.3)(-0.9) teragrams of carbon per year from the Mackenzie River, which is three times the CO2 drawdown by silicate weathering in this basin. Offshore, we find evidence for efficient terrestrial organic carbon burial over the Holocene period, suggesting that erosion of organic carbon-rich, high-latitude soils may result in an important geological CO2 sink.

The oxidation of organic carbon contained within sedimentary rocks ("petrogenic" carbon, or hereafter OCpetro) emits nearly as much C2 as is released by volcanism, thereby playing a key role in the long-term global C budget. High erosion rates in mountains have been shown to increase OCpetro oxidation. However, these settings also export unweathered material that may continue to react in downstream floodplains. The relative importance of OCpetro oxidation in mountains versus floodplains remains difficult to assess as disparate methods have been used in the different environments. Here, we investigate the sources and fluxes of rhenium (Re) in the Rio Madre de Dios to quantify OCpetro oxidation from the Andes to the Amazon floodplain using a common approach. Dissolved rhenium concentrations (n = 131) range from 0.01 to 63 pmol L-1 and vary depending on lithology and geomorphic setting. We find that >75% of the dissolved Re derives from OCpetro oxidation and that this proportion increases downstream. We estimate that in the Andes, OCpetro oxidation releases 11.2+4.5/-2.8 tC km-2 y-1 of C2, which corresponds to ~41% of the total OCpetro denudation (sum of oxidized and solid OCpetro). A Re mass balance across the Rio Madre de Dios shows that 46% of OCpetro oxidation takes place in the Andes, 14% in the foreland-lowlands, and 40% in the Andean-fed floodplains. This doubling of OCpetro oxidation flux downstream of the Andes demonstrates that, when present, floodplains can greatly increase OCpetro oxidation and C2 release. [ABSTRACT FROM AUTHOR]

Seawater lithium isotopes (δ7Li) record changes over Earth history, including a ∼9‰ increase during the Cenozoic interpreted as reflecting either a change in continental silicate weathering rate or weathering feedback strength, associated with tectonic uplift. However, mechanisms controlling the dissolved δ7Li remain debated. Here we report time-series δ7Li measurements from Tibetan and Pamir rivers, and combine them with published seasonal data, covering small (<102 km2) to large rivers (>106 km2). We find seasonal changes in δ7Li across all latitudes: dry seasons consistently have higher δ7Li than wet seasons, by −0.3‰ to 16.4‰ (mean 5.0 ± 2.5‰). A globally negative correlation between δ7Li and annual runoff reflects the hydrological intensity operating in catchments, regulating water residence time and δ7Li values. This hydrological control on δ7Li is consistent across climate events back to ~445 Ma. We propose that hydrological changes result in shifts in river δ7Li and urge reconsideration of its use to examine past weathering intensity and flux, opening a new window to reconstruct hydrological conditions. From modern seasonal to the deep time, global data show that continental hydrology has a direct and consistent effect on river and marine Li isotope compositions, highlighting a crucial role of climate on Earth's weathering and the carbon cycle. [ABSTRACT FROM AUTHOR]

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 2018Export of aged DOC is consistent with a prolonged warming period and the formation of supra‐permafrost taliksMobilization of aged DOC and nitrate suggests percolation of supra‐permafrost groundwater through previously frozen soil layers [ABSTRACT FROM AUTHOR]

Erosion drives the export of particulate organic carbon from the terrestrial biosphere (POC biosphere ) and its delivery to rivers. The carbon transfer is globally significant and can result in drawdown of atmospheric carbon dioxide (CO 2 ) if the eroded POC biosphere escapes degradation during river transfer and sedimentary deposition. Despite this recognition, we lack a global perspective on how the tectonic and climatic factors which govern physical erosion regulate POC biosphere discharge, obscuring linkages between mountain building, climate, and CO 2 drawdown. To fill this deficit, geochemical (δ 13 C, 14 C and C/N), hydrometric (water discharge, suspended sediment concentration) and geomorphic (slope) measurements are combined from 33 globally-distributed forested mountain catchments. Radiocarbon activity is used to account for rock-derived organic carbon and reveals that POC biosphere eroded from mountain forests is mostly < 1300 14 C years old. Annual POC biosphere yields are positively correlated with suspended sediment yields, confirming results from Taiwan and a recent global analysis, and are high in catchments with the steepest slopes. Based on these relationships and the global distribution of slope angles (3-arc-second), it is suggested that topography steeper than 10° (16% of the continental area) may contribute ~ 40% of global POC biosphere erosional flux. Climate is shown to regulate POC biosphere discharge by mountain rivers, by controlling hydrologically-driven erosion processes. In catchments where discharge measurements are available (8 of the 33) a significant relationship exists between daily runoff (mm day − 1 ) and POC biosphere concentration (mg L − 1 ) ( r = 0.53, P < 0.0001). The relationship can be described by a single power law and suggests a high connectivity between forested hillslopes and mountain river channels. As a result, annual POC biosphere yields are significantly correlated with mean annual runoff ( r = 0.64, P < 0.0001). A shear-stress POC biosphere erosion model is proposed which can explain the patterns in the data. The model allows the climate sensitivity of this carbon flux to be assessed for the first time. For a 1% increase in annual runoff, POC biosphere discharge is predicted to increase by ~ 4%. In steeper catchments, POC biosphere discharge increases more rapidly with an increase in annual runoff. For comparison, a 1% increase in annual runoff is predicted to increase carbon transfers by silicate weathering solute fluxes in mountains by 0.4–0.7%. Depending on the fate of the eroded POC biosphere , river export of POC biosphere from mountains may act as an important negative feedback on rising atmospheric CO 2 and increased global temperature. Erosion of carbon from the terrestrial biosphere links mountain building and climate to the geological evolution of atmospheric CO 2 , while the carbon fluxes are sensitive to predicted changes in runoff over the coming century. [ABSTRACT FROM AUTHOR]

Mineral weathering plays a primary role in the geologic carbon cycle. Silicate weathering by carbonic acid consumes CO² and stabilizes Earth's climate system. However, when sulfuric acid drives weathering, CO² can be released to the atmosphere. Recent work has established that sulfuric acid weathering resulting from sulfide mineral oxidation is globally significant and particularly important in rapidly eroding environments. In contrast, if SO4 ²-produced by sulfide oxidation is reduced during continental transit, then CO² release may be negated. Yet, little is known about how much SO4 ²-reduction takes place in terrestrial environments. We report oxygen and sulfur stable isotope ratios of SO4 ²-in river waters and mass budget calculations, which together suggest that SO4 ²-released from pyrite oxidation in the Peruvian Andes mountains is conservatively exported across ~300 km of the Amazon floodplain. In this system, floodplain SO4 ²-reduction does not counteract the large SO4 ²-flux from Andean pyrite weathering or measurably affect the stable isotope composition of riverine SO4 ²-. These findings support the hypothesis that uplift and erosion of sedimentary rocks drive release of CO² from the rock reservoir to the atmosphere. [ABSTRACT FROM AUTHOR]