McClelland
James W.
McClelland
James W.
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ArticleIsotopic signals (18O, 2H, 3H) of six major rivers draining the pan-Arctic watershed(American Geophysical Union, 2012-03-22) Yi, Y. ; Gibson, J. J. ; Cooper, Lee W. ; Helie, J.-F. ; Birks, S. J. ; McClelland, James W. ; Holmes, Robert M. ; Peterson, Bruce J.We present the results of a 4-year collaborative sampling effort that measured δ18O, δ2H values and 3H activities in the six largest Arctic rivers (the Ob, Yenisey, Lena, Kolyma, Yukon and Mackenzie). Using consistent sampling and data processing protocols, these isotopic measurements provide the best available δ2H and 3H estimates for freshwater fluxes from the pan-Arctic watershed to the Arctic Ocean and adjacent seas, which complements previous efforts with δ18O and other tracers. Flow-weighted annual δ2H values vary from −113.3‰ to −171.4‰ among rivers. Annual 3H fluxes vary from 0.68 g to 4.12 g among basins. The integration of conventional hydrological and landscape observations with stable water isotope signals, and estimation of areal yield of 3H provide useful insights for understanding water sources, mixing and evaporation losses in these river basins. For example, an inverse correlation between the slope of the δ18O-δ2H relation and wetland extent indicates that wetlands play comparatively important roles affecting evaporation losses in the Yukon and Mackenzie basins. Tritium areal yields (ranging from 0.760 to 1.695 10−6 g/km2 per year) are found to be positively correlated with permafrost coverage within the studied drainage basins. Isotope-discharge relationships demonstrate both linear and nonlinear response patterns, which highlights the complexity of hydrological processes in large Arctic river basins. These isotope observations and their relationship to discharge and landscape features indicate that basin-specific characteristics significantly influence hydrological processes in the pan-Arctic watershed.
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ArticleRiver export of nutrients and organic matter from the North Slope of Alaska to the Beaufort Sea(John Wiley & Sons, 2014-02-28) McClelland, James W. ; Townsend-Small, Amy ; Holmes, Robert M. ; Pan, Feifei ; Stieglitz, Marc ; Khosh, Matt ; Peterson, Bruce J.While river-borne materials are recognized as important resources supporting coastal ecosystems around the world, estimates of river export from the North Slope of Alaska have been limited by a scarcity of water chemistry and river discharge data. This paper quantifies water, nutrient, and organic matter export from the three largest rivers (Sagavanirktok, Kuparuk, and Colville) that drain Alaska's North Slope and discusses the potential importance of river inputs for biological production in coastal waters of the Alaskan Beaufort Sea. Together these rivers export ∼297,000 metric tons of organic carbon and ∼18,000 metric tons of organic nitrogen each year. Annual fluxes of nitrate-N, ammonium-N, and soluble reactive phosphorus are approximately 1750, 200, and 140 metric tons per year, respectively. Constituent export from Alaska's North Slope is dominated by the Colville River. This is in part due to its larger size, but also because constituent yields are greater in the Colville watershed. River-supplied nitrogen may be more important to productivity along the Alaskan Beaufort Sea coast than previously thought. However, given the dominance of organic nitrogen export, the potential role of river-supplied nitrogen in support of primary production depends strongly on remineralization mechanisms. Although rivers draining the North Slope of Alaska make only a small contribution to overall river export from the pan-arctic watershed, comparisons with major arctic rivers reveal unique regional characteristics as well as remarkable similarities among different regions and scales. Such information is crucial for development of robust river export models that represent the arctic system as a whole.
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ArticleThe processing and impact of dissolved riverine nitrogen in the Arctic Ocean(Springer, 2011-06-11) Tank, Suzanne E. ; Manizza, Manfredi ; Holmes, Robert M. ; McClelland, James W. ; Peterson, Bruce J.Although the Arctic Ocean is the most riverine-influenced of all of the world’s oceans, the importance of terrigenous nutrients in this environment is poorly understood. This study couples estimates of circumpolar riverine nutrient fluxes from the PARTNERS (Pan-Arctic River Transport of Nutrients, Organic Matter, and Suspended Sediments) Project with a regionally configured version of the MIT general circulation model to develop estimates of the distribution and availability of dissolved riverine N in the Arctic Ocean, assess its importance for primary production, and compare these estimates to potential bacterial production fueled by riverine C. Because riverine dissolved organic nitrogen is remineralized slowly, riverine N is available for uptake well into the open ocean. Despite this, we estimate that even when recycling is considered, riverine N may support 0.5–1.5 Tmol C year−1 of primary production, a small proportion of total Arctic Ocean photosynthesis. Rapid uptake of dissolved inorganic nitrogen coupled with relatively high rates of dissolved organic nitrogen regeneration in N-limited nearshore regions, however, leads to potential localized rates of riverine-supported photosynthesis that represent a substantial proportion of nearshore production.
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PreprintAn analysis of the carbon balance of the Arctic Basin from 1997 to 2006( 2010-06-18) McGuire, A. David ; Hayes, Daniel J. ; Kicklighter, David W. ; Manizza, Manfredi ; Zhuang, Qianlai ; Chen, Min ; Follows, Michael J. ; Gurney, Kevin R. ; McClelland, James W. ; Melillo, Jerry M. ; Peterson, Bruce J. ; Prinn, Ronald G.This study used several model-based tools to analyze the dynamics of the Arctic Basin between 1997 and 2006 as a linked system of land-ocean-atmosphere C exchange. The analysis estimates that terrestrial areas of the Arctic Basin lost 62.9 Tg C yr-1 and that the Arctic Ocean gained 94.1 Tg C yr-1. Arctic lands and oceans were a net CO2 sink of 108.9 Tg C yr-1, which is within the range of uncertainty in estimates from atmospheric inversions. Although both lands and oceans of the Arctic were estimated to be CO2 sinks, the land sink diminished in strength because of increased fire disturbance compared to previous decades, while the ocean sink increased in strength because of increased biological pump activity associated with reduced sea ice cover. Terrestrial areas of the Arctic were a net source of 41.5 Tg CH4 yr-1 that increased by 0.6 Tg CH4 yr-1 during the decade of analysis, a magnitude that is comparable with an atmospheric inversion of CH4. Because the radiative forcing of the estimated CH4 emissions is much greater than the CO2 sink, the analysis suggests that the Arctic Basin is a substantial net source of green house gas forcing to the climate system.
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DatasetChemical data associated with field collections from the Gulf of Maine, Nauset Marsh Estuary System, and Long Island Sound (Alexandrium isotopes project)(Biological and Chemical Oceanography Data Management Office (BCO-DMO). Contact: bco-dmo-data@whoi.edu, 2019-03-20) Smith, Juliette L. ; Anderson, Donald M. ; Erdner, Deana L. ; McClelland, James W.Chemical data associated with field collections from the Gulf of Maine, Nauset Marsh Estuary System, and Long Island Sound (Alexandrium isotopes project) For a complete list of measurements, refer to the full dataset description in the supplemental file 'Dataset_description.pdf'. The most current version of this dataset is available at: https://www.bco-dmo.org/dataset/712027
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PreprintSeasonal and annual fluxes of nutrients and organic matter from large rivers to the Arctic Ocean and surrounding seas( 2011-03) Holmes, Robert M. ; McClelland, James W. ; Peterson, Bruce J. ; Tank, Suzanne E. ; Bulygina, Ekaterina ; Eglinton, Timothy I. ; Gordeev, Viacheslav V. ; Gurtovaya, Tatiana Y. ; Raymond, Peter A. ; Repeta, Daniel J. ; Staples, Robin ; Striegl, Robert G. ; Zhulidov, Alexander V. ; Zimov, Sergey A.River inputs of nutrients and organic matter impact the biogeochemistry of arctic estuaries and the Arctic Ocean as a whole, yet there is considerable uncertainty about the magnitude of fluvial fluxes at the pan-arctic scale. Samples from the six largest arctic rivers, with a combined watershed area of 11.3 x 106 km2, have revealed strong seasonal variations in constituent concentrations and fluxes within rivers as well as large differences among the rivers. Specifically, we investigate fluxes of dissolved organic carbon, dissolved organic nitrogen, total dissolved phosphorus, dissolved inorganic nitrogen, nitrate, and silica. This is the first time that seasonal and annual constituent fluxes have been determined using consistent sampling and analytical methods at the pan arctic scale, and consequently provide the best available estimates for constituent flux from land to the Arctic Ocean and surrounding seas. Given the large inputs of river water to the relatively small Arctic Ocean, and the dramatic impacts that climate change is having in the Arctic, it is particularly urgent that we establish the contemporary river fluxes so that we will be able to detect future changes and evaluate the impact of the changes on the biogeochemistry of the receiving coastal and ocean systems.
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ArticleBiomass offsets little or none of permafrost carbon release from soils, streams, and wildfire : an expert assessment(IOPScience, 2016-03-07) Abbott, Benjamin W. ; Jones, Jeremy B. ; Schuur, Edward A. G. ; Chapin, F. Stuart ; Bowden, William B. ; Bret-Harte, M. Syndonia ; Epstein, Howard E. ; Flannigan, Michael ; Harms, Tamara K. ; Hollingsworth, Teresa N. ; Mack, Michelle C. ; McGuire, A. David ; Natali, Susan M. ; Rocha, Adrian V. ; Tank, Suzanne E. ; Turetsky, Merritt R. ; Vonk, Jorien E. ; Wickland, Kimberly ; Aiken, George R. ; Alexander, Heather D. ; Amon, Rainer M. W. ; Benscoter, Brian ; Bergeron, Yves ; Bishop, Kevin ; Blarquez, Olivier ; Bond-Lamberty, Benjamin ; Breen, Amy L. ; Buffam, Ishi ; Cai, Yihua ; Carcaillet, Christopher ; Carey, Sean K. ; Chen, Jing M. ; Chen, Han Y. H. ; Christensen, Torben R. ; Cooper, Lee W. ; Cornelissen, Johannes H. C. ; de Groot, William J. ; DeLuca, Thomas Henry ; Dorrepaal, Ellen ; Fetcher, Ned ; Finlay, Jacques C. ; Forbes, Bruce C. ; French, Nancy H. F. ; Gauthier, Sylvie ; Girardin, Martin ; Goetz, Scott J. ; Goldammer, Johann G. ; Gough, Laura ; Grogan, Paul ; Guo, Laodong ; Higuera, Philip E. ; Hinzman, Larry ; Hu, Feng Sheng ; Hugelius, Gustaf ; JAFAROV, ELCHIN ; Jandt, Randi ; Johnstone, Jill F. ; Karlsson, Jan ; Kasischke, Eric S. ; Kattner, Gerhard ; Kelly, Ryan ; Keuper, Frida ; Kling, George W. ; Kortelainen, Pirkko ; Kouki, Jari ; Kuhry, Peter ; Laudon, Hjalmar ; Laurion, Isabelle ; Macdonald, Robie W. ; Mann, Paul J. ; Martikainen, Pertti ; McClelland, James W. ; Molau, Ulf ; Oberbauer, Steven F. ; Olefeldt, David ; Paré, David ; Parisien, Marc-André ; Payette, Serge ; Peng, Changhui ; Pokrovsky, Oleg ; Rastetter, Edward B. ; Raymond, Peter A. ; Raynolds, Martha K. ; Rein, Guillermo ; Reynolds, James F. ; Robards, Martin ; Rogers, Brendan ; Schädel, Christina ; Schaefer, Kevin ; Schmidt, Inger K. ; Shvidenko, Anatoly ; Sky, Jasper ; Spencer, Robert G. M. ; Starr, Gregory ; Striegl, Robert ; Teisserenc, Roman ; Tranvik, Lars J. ; Virtanen, Tarmo ; Welker, Jeffrey M. ; Zimov, Sergey A.As the permafrost region warms, its large organic carbon pool will be increasingly vulnerable to decomposition, combustion, and hydrologic export. Models predict that some portion of this release will be offset by increased production of Arctic and boreal biomass; however, the lack of robust estimates of net carbon balance increases the risk of further overshooting international emissions targets. Precise empirical or model-based assessments of the critical factors driving carbon balance are unlikely in the near future, so to address this gap, we present estimates from 98 permafrost-region experts of the response of biomass, wildfire, and hydrologic carbon flux to climate change. Results suggest that contrary to model projections, total permafrost-region biomass could decrease due to water stress and disturbance, factors that are not adequately incorporated in current models. Assessments indicate that end-of-the-century organic carbon release from Arctic rivers and collapsing coastlines could increase by 75% while carbon loss via burning could increase four-fold. Experts identified water balance, shifts in vegetation community, and permafrost degradation as the key sources of uncertainty in predicting future system response. In combination with previous findings, results suggest the permafrost region will become a carbon source to the atmosphere by 2100 regardless of warming scenario but that 65%–85% of permafrost carbon release can still be avoided if human emissions are actively reduced.
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ArticleA land-to-ocean perspective on the magnitude, source and implication of DIC flux from major Arctic rivers to the Arctic Ocean(American Geophysical Union, 2012-12-14) Tank, Suzanne E. ; Raymond, Peter A. ; Striegl, Robert G. ; McClelland, James W. ; Holmes, Robert M. ; Fiske, Gregory J. ; Peterson, Bruce J.A series of seasonally distributed measurements from the six largest Arctic rivers (the Ob', Yenisey, Lena, Kolyma, Yukon and Mackenzie) was used to examine the magnitude and significance of Arctic riverine DIC flux to larger scale C dynamics within the Arctic system. DIC concentration showed considerable, and synchronous, seasonal variation across these six large Arctic rivers, which have an estimated combined annual DIC flux of 30 Tg C yr−1. By examining the relationship between DIC flux and landscape variables known to regulate riverine DIC, we extrapolate to a DIC flux of 57 ± 9.9 Tg C yr−1for the full pan-arctic basin, and show that DIC export increases with runoff, the extent of carbonate rocks and glacial coverage, but decreases with permafrost extent. This pan-arctic riverine DIC estimate represents 13–15% of the total global DIC flux. The annual flux of selected ions (HCO3−, Na+, Ca2+, Mg2+, Sr2+, and Cl−) from the six largest Arctic rivers confirms that chemical weathering is dominated by inputs from carbonate rocks in the North American watersheds, but points to a more important role for silicate rocks in Siberian watersheds. In the coastal ocean, river water-induced decreases in aragonite saturation (i.e., an ocean acidification effect) appears to be much more pronounced in Siberia than in the North American Arctic, and stronger in the winter and spring than in the late summer. Accounting for seasonal variation in the flux of DIC and other major ions gives a much clearer understanding of the importance of riverine DIC within the broader pan-arctic C cycle.
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ArticleParticulate organic carbon and nitrogen export from major Arctic rivers(John Wiley & Sons, 2016-05-11) McClelland, James W. ; Holmes, Robert M. ; Peterson, Bruce J. ; Raymond, Peter A. ; Striegl, Robert ; Zhulidov, Alexander V. ; Zimov, Sergey A. ; Zimov, Nikita ; Tank, Suzanne E. ; Spencer, Robert G. M. ; Staples, Robin ; Gurtovaya, Tatiana Y. ; Griffin, Claire G.Northern rivers connect a land area of approximately 20.5 million km2 to the Arctic Ocean and surrounding seas. These rivers account for ~10% of global river discharge and transport massive quantities of dissolved and particulate materials that reflect watershed sources and impact biogeochemical cycling in the ocean. In this paper, multiyear data sets from a coordinated sampling program are used to characterize particulate organic carbon (POC) and particulate nitrogen (PN) export from the six largest rivers within the pan-Arctic watershed (Yenisey, Lena, Ob', Mackenzie, Yukon, Kolyma). Together, these rivers export an average of 3055 × 109 g of POC and 368 × 109 g of PN each year. Scaled up to the pan-Arctic watershed as a whole, fluvial export estimates increase to 5767 × 109 g and 695 × 109 g of POC and PN per year, respectively. POC export is substantially lower than dissolved organic carbon export by these rivers, whereas PN export is roughly equal to dissolved nitrogen export. Seasonal patterns in concentrations and source/composition indicators (C:N, δ13C, Δ14C, δ15N) are broadly similar among rivers, but distinct regional differences are also evident. For example, average radiocarbon ages of POC range from ~2000 (Ob') to ~5500 (Mackenzie) years before present. Rapid changes within the Arctic system as a consequence of global warming make it challenging to establish a contemporary baseline of fluvial export, but the results presented in this paper capture variability and quantify average conditions for nearly a decade at the beginning of the 21st century.
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ArticleSeasonal and hydrologic drivers of dissolved organic matter and nutrients in the upper Kuparuk River, Alaskan Arctic(Springer, 2010-05-08) Townsend-Small, Amy ; McClelland, James W. ; Holmes, Robert M. ; Peterson, Bruce J.As the planet warms, widespread changes in Arctic hydrology and biogeochemistry have been documented and these changes are expected to accelerate in the future. Improved understanding of the behavior of water-borne constituents in Arctic rivers with varying hydrologic conditions, including seasonal variations in discharge–concentration relationships, will improve our ability to anticipate future changes in biogeochemical budgets due to changing hydrology. We studied the relationship between seasonal water discharge and dissolved organic carbon and nitrogen (DOC and DON) and nutrient concentrations in the upper Kuparuk River, Arctic Alaska. Fluxes of most constituents were highest during initial snowmelt runoff in spring, indicating that this historically under-studied period contributes significantly to total annual export. In particular, the initial snowmelt period (the stream is completely frozen during the winter) accounted for upwards of 35% of total export of DOC and DON estimated for the entire study period. DOC and DON concentrations were positively correlated with discharge whereas nitrate (NO3 −) and silicate were negatively correlated with discharge throughout the study. However, discharge-specific DOC and DON concentrations (i.e. concentrations compared at the same discharge level) decreased over the summer whereas discharge-specific concentrations of NO3 − and silicate increased. Soluble reactive phosphorus (SRP) and ammonium (NH4 +) were negatively correlated with discharge during the spring thaw, but were less predictable with respect to discharge thereafter. These data provide valuable information on how Arctic watershed biogeochemistry will be affected by future changes in temperature, snowfall, and rainfall in the Arctic. In particular, our results add to a growing body of research showing that nutrient export per unit of stream discharge, particularly NO3 −, is increasing in the Arctic.
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ArticleInsights and issues with simulating terrestrial DOC loading of Arctic river networks(Ecological Society of America, 2013-12) Kicklighter, David W. ; Hayes, Daniel J. ; McClelland, James W. ; Peterson, Bruce J. ; McGuire, A. David ; Melillo, Jerry M.Terrestrial carbon dynamics influence the contribution of dissolved organic carbon (DOC) to river networks in addition to hydrology. In this study, we use a biogeochemical process model to simulate the lateral transfer of DOC from land to the Arctic Ocean via riverine transport. We estimate that, over the 20th century, the pan-Arctic watershed has contributed, on average, 32 Tg C/yr of DOC to river networks emptying into the Arctic Ocean with most of the DOC coming from the extensive area of boreal deciduous needle-leaved forests and forested wetlands in Eurasian watersheds. We also estimate that the rate of terrestrial DOC loading has been increasing by 0.037 Tg C/yr2 over the 20th century primarily as a result of climate-induced increases in water yield. These increases have been offset by decreases in terrestrial DOC loading caused by wildfires. Other environmental factors (CO2 fertilization, ozone pollution, atmospheric nitrogen deposition, timber harvest, agriculture) are estimated to have relatively small effects on terrestrial DOC loading to Arctic rivers. The effects of the various environmental factors on terrestrial carbon dynamics have both offset and enhanced concurrent effects on hydrology to influence terrestrial DOC loading and may be changing the relative importance of terrestrial carbon dynamics on this carbon flux. Improvements in simulating terrestrial DOC loading to pan-Arctic rivers in the future will require better information on the production and consumption of DOC within the soil profile, the transfer of DOC from land to headwater streams, the spatial distribution of precipitation and its temporal trends, carbon dynamics of larch-dominated ecosystems in eastern Siberia, and the role of industrial organic effluents on carbon budgets of rivers in western Russia.
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ArticleLandscape-level controls on dissolved carbon flux from diverse catchments of the circumboreal(American Geophysical Union, 2012-08-21) Tank, Suzanne E. ; Frey, Karen E. ; Striegl, Robert G. ; Raymond, Peter A. ; Holmes, Robert M. ; McClelland, James W. ; Peterson, Bruce J.While much of the dissolved organic carbon (DOC) within rivers is destined for mineralization to CO2, a substantial fraction of riverine bicarbonate (HCO3−) flux represents a CO2 sink, as a result of weathering processes that sequester CO2 as HCO3−. We explored landscape-level controls on DOC and HCO3− flux in subcatchments of the boreal, with a specific focus on the effect of permafrost on riverine dissolved C flux. To do this, we undertook a multivariate analysis that partitioned the variance attributable to known, key regulators of dissolved C flux (runoff, lithology, and vegetation) prior to examining the effect of permafrost, using riverine biogeochemistry data from a suite of subcatchments drawn from the Mackenzie, Yukon, East, and West Siberian regions of the circumboreal. Across the diverse catchments that we study, controls on HCO3− flux were near-universal: runoff and an increased carbonate rock contribution to weathering (assessed as riverwater Ca:Na) increased HCO3− yields, while increasing permafrost extent was associated with decreases in HCO3−. In contrast, permafrost had contrasting and region-specific effects on DOC yield, even after the variation caused by other key drivers of its flux had been accounted for. We used ionic ratios and SO4 yields to calculate the potential range of CO2 sequestered via weathering across these boreal subcatchments, and show that decreasing permafrost extent is associated with increases in weathering-mediated CO2 fixation across broad spatial scales, an effect that could counterbalance some of the organic C mineralization that is predicted with declining permafrost.
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ArticleA model of the Arctic Ocean carbon cycle(American Geophysical Union, 2011-12-15) Manizza, Manfredi ; Follows, Michael J. ; Dutkiewicz, Stephanie ; Menemenlis, Dimitris ; McClelland, James W. ; Hill, C. N. ; Peterson, Bruce J. ; Key, Robert M.A three dimensional model of Arctic Ocean circulation and mixing, with a horizontal resolution of 18 km, is overlain by a biogeochemical model resolving the physical, chemical and biological transport and transformations of phosphorus, alkalinity, oxygen and carbon, including the air-sea exchange of dissolved gases and the riverine delivery of dissolved organic carbon. The model qualitatively captures the observed regional and seasonal trends in surface ocean PO4, dissolved inorganic carbon, total alkalinity, and pCO2. Integrated annually, over the basin, the model suggests a net annual uptake of 59 Tg C a−1, within the range of published estimates based on the extrapolation of local observations (20–199 Tg C a−1). This flux is attributable to the cooling (increasing solubility) of waters moving into the basin, mainly from the subpolar North Atlantic. The air-sea flux is regulated seasonally and regionally by sea-ice cover, which modulates both air-sea gas transfer and the photosynthetic production of organic matter, and by the delivery of riverine dissolved organic carbon (RDOC), which drive the regional contrasts in pCO2 between Eurasian and North American coastal waters. Integrated over the basin, the delivery and remineralization of RDOC reduces the net oceanic CO2 uptake by ~10%.
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PreprintSulfur isotopes in rivers : insights into global weathering budgets, pyrite oxidation, and the modern sulfur cycle( 2018-05) Burke, Andrea ; Present, Theodore M. ; Paris, Guillaume ; Rae, Emily C. M. ; Sandilands, Brodie H. ; Gaillardet, Jerome ; Peucker-Ehrenbrink, Bernhard ; Fischer, Woodward W. ; McClelland, James W. ; Spencer, Robert G. M. ; Voss, Britta M. ; Adkins, Jess F.The biogeochemical sulfur cycle is intimately linked to the cycles of carbon, iron, and oxygen, and plays an important role in global climate via weathering reactions and aerosols. However, many aspects of the modern budget of the global sulfur cycle are not fully understood. We present new δ34S measurements on sulfate from more than 160 river samples from different geographical and climatic regions—more than 46% of the world’s freshwater flux to the ocean is accounted for in this estimate of the global riverine sulfur isotope budget. These measurements include major rivers and their tributaries, as well as time series, and are combined with previously published data to estimate the modern flux-weighted global riverine δ34S as 4.4 ± 4.5 ‰ (V-CDT), and 4.8 ± 4.9 ‰ when the most polluted rivers are excluded. Combined with major anion and cation concentrations, the sulfur isotope data allow us to tease apart the relative contributions of different processes to the modern riverine sulfur budget, resulting in new estimates of the flux of riverine sulfate due to the oxidative weathering of pyrites (1.3 ± 0.2 Tmol S/y) and the weathering of sedimentary sulfate minerals (1.5 ± 0.2 Tmol S/y). These data indicate that previous estimates of the global oxidative weathering of pyrite have been too low by a factor of two. As pyrite oxidation coupled to carbonate weathering can act as a source of CO2 to the atmosphere, this global pyrite weathering budget implies that the global CO2 weathering sink is overestimated. Furthermore, the large range of sulfur isotope ratios in modern rivers indicates that secular changes in the lithologies exposed to weathering through time could play a major role in driving past variations in δ34S of seawater.