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Glacial Weathering, Sulfide Oxidation, and Global Carbon Cycle Feedbacks

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Glacial Weathering, Sulfide Oxidation, and Global Carbon Cycle Feedbacks Glacial weathering, sulfide oxidation, and global carbon cycle feedbacks Mark A. Torresa,b,c,1, Nils Moosdorfa,d,e,1, Jens Hartmannd, Jess F. Adkinsb, and A. Joshua Westa,2 aDepartment of Earth Sciences, University of Southern California, Los Angeles, CA 90089; bDivision of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA 91125; cDepartment of Earth, Environmental, and Planetary Sciences, Rice University, Houston, TX 77005; dInstitute for Geology, Center for Earth System Research and Sustainability (CEN), Universität Hamburg, 20146 Hamburg, Germany; and eLeibniz Center for Tropical Marine Research, 28359 Bremen, Germany Edited by Thure E. Cerling, University of Utah, Salt Lake City, UT, and approved July 5, 2017 (received for review February 21, 2017) Connections between glaciation, chemical weathering, and the global erosion (5, 8, 9), which is thought to promote more rapid silicate carbon cycle could steer the evolution of global climate over geologic weathering (10, 11). If glaciation increases erosion rates, and if time, but even the directionality of feedbacks in this system remain to erosion enhances silicate weathering and associated production of be resolved. Here, we assemble a compilation of hydrochemical data alkalinity, then glacial weathering could act as a positive feedback from glacierized catchments, use this data to evaluate the dominant serving to promote further glaciation (5, 12). chemical reactions associated with glacial weathering, and explore the Glaciation may also affect rates of weathering of nonsilicate implications for long-term geochemical cycles. Weathering yields from minerals. Studies of glacial hydrochemistry have pointed to the im- catchments in our compilation are higher than the global average, portance of sulfide oxidation and carbonate dissolution as major which results, in part, from higher runoff in glaciated catchments. solute sources (13–15). Because the residence time of sulfate in the Our analysis supports the theory that glacial weathering is character- oceans is long relative to Ca, sulfide–carbonate weathering can act to ized predominantly by weathering of trace sulfide and carbonate min- release CO2 to the ocean–atmosphere system over timescales erals. To evaluate the effects of glacial weathering on atmospheric of <100 My (16, 17). Sulfide oxidation also influences global budgets pCO2, we use a solute mixing model to predict the ratio of alkalinity of redox-sensitive elements including sulfur, iron, and oxygen (16, 18, to dissolved inorganic carbon (DIC) generated by weathering reactions. 19). Although sulfide and carbonate minerals are usually present at Compared with nonglacial weathering, glacial weathering is more low abundance in most rocks, their rates of dissolution are typically likely to yield alkalinity/DIC ratios less than 1, suggesting that enhanced EARTH, ATMOSPHERIC, orders of magnitude faster than for silicate minerals. For example, AND PLANETARY SCIENCES sulfide oxidation as a result of glaciation may act as a source of CO2 to log rates from laboratory experiments are −6to−10 for pyrite (20), the atmosphere. Back-of-the-envelope calculations indicate that oxida- vs. log rates of −10 to −16 for silicate minerals (21). Thus, even a tive fluxes could change ocean–atmosphere CO2 equilibrium by 25 ppm small proportion of sulfide or carbonate present in rocks can dom- or more over 10 ky. Over longer timescales, CO2 release could act as a inate solute production (22, 23). Indeed, weathering of these trace negative feedback, limiting progress of glaciation, dependent on lithol- phases is predominantly “supply limited” in the present day, so fluxes ogy and the concentration of atmospheric O2. Future work on glacia- increase with erosion that supplies more minerals for reaction (17, tion–weathering–carbon cycle feedbacks should consider weathering 24). In contrast, silicate weathering is not always limited by supply of of trace sulfide minerals in addition to silicate minerals. weatherable minerals (25). As a result, if glaciation enhances phys- ical erosion rates, the increased exposure of fresh rock material weathering | carbon cycle | glaciation | oxidation | sulfide containing unweathered minerals should drive increased sulfide and carbonate weathering fluxes, but may not drive increased silicate pisodes of glaciation represent some of the most dramatic weathering fluxes in tandem. Thus, the net effect of glaciation could Echanges in the history of Earth’s climate. Basic questions be to supply CO2 to the atmosphere, rather than to remove it. remain unanswered about why the planet has occasionally but not always supported glaciers, about why some glaciations have been Significance more intense than others, and about how glaciers have shaped Earth’s landscapes, chemical cycles, and climate. Before the Phan- We compile data showing that, as hypothesized previously, waters erozoic (i.e., before ∼540 Mya), several glaciations are thought to draining glaciers have solute chemistry that is distinct from non- have approached complete or near-complete planetary ice cover glacial rivers and reflects different proportions of mineral weath- (“Snowball Earth” events; ref. 1). In contrast, more recent glacia- ering reactions. Elevated pyrite oxidation during glacial weathering tions, including the Quaternary glaciations of the last million years, could generate acidity, releasing carbon to the atmosphere. We have been characterized by oscillating climate with ice extent lim- show that this effect could contribute to changes in CO2 during ited to high latitudes even during glacial maxima (2). The formation glacial cycles of the past million years. Over the longer, multimillion- of ice cover has long been known to fundamentally alter Earth’s year timescales that Earth transitions into and out of glaciated environment, changing albedo (3), influencing atmospheric and states, sustained addition of pyrite-derived sulfate to the oceans ocean circulation (4), and reshaping landscapes (5). These diverse could shift the balance of the global carbon cycle toward increasing – effects may contribute to planetary-scale feedbacks that influence CO2 in the ocean atmosphere, thus providing a negative-feedback the transition to and the evolution of glaciation. mechanism preventing runaway glaciation. This mechanism de- Chemical weathering influences the composition of the atmo- pends on oxidation and thus sufficient O2. sphere by releasing ionic species from minerals that alter the al- – Author contributions: N.M., J.H., and A.J.W. designed research; M.A.T., N.M., and J.H. kalinity and redox condition of the ocean atmosphere system. performed research; M.A.T. and J.F.A. contributed new reagents/analytic tools; M.A.T., Weathering of silicate minerals produces alkalinity, removing N.M., J.H., J.F.A., and A.J.W. analyzed data; and M.A.T. and A.J.W. wrote the paper. carbon from the atmosphere in the process (6). If glaciers reduce The authors declare no conflict of interest. weathering fluxes from land area that was previously undergoing This article is a PNAS Direct Submission. silicate weathering, glaciation may decrease global alkalinity pro- 1M.A.T. and N.M. contributed equally to this work. duction, allow atmospheric CO2 levels to rise, and thus generate a 2To whom correspondence should be addressed. Email: [email protected]. negative feedback that ends glaciation (7). On the other hand, This article contains supporting information online at www.pnas.org/lookup/suppl/doi:10. some evidence suggests that glaciation increases rates of physical 1073/pnas.1702953114/-/DCSupplemental. www.pnas.org/cgi/doi/10.1073/pnas.1702953114 PNAS Early Edition | 1of6 Downloaded by guest on October 1, 2021 The directionality of long-term glaciation–weathering feed- proportion of glacial cover and the sampling distance from the backs depends on the extent to which glacial weathering is a net glacial snout (SI Appendix,TableS3). Subglacial weathering fluxes source or net sink of CO2 to the atmosphere, which in turn de- also depend on hydrology, for example, differing for warm- vs. cold- pends on the balance of sulfide vs. silicate mineral weathering. A based ice (35, 36) and along different flowpaths (37), and these growing number of studies have explored various aspects of differences may explain some of the variability within the dataset. glacial weathering by analyzing the chemical composition of glacial runoff, often focusing on specific case studies, and in Distinct Stoichiometry of Glacial Weathering. Our compilation provides some cases synthesizing global datasets (13, 26, 27). Here, we the opportunity to test the hypothesis that the solute stoichiometry assemble an expanded compilation of glacial weathering data of glaciated rivers is distinct from nonglaciated rivers, because the and use this compilation to identify characteristic features of large number of data points allows for statistical comparison be- present-day glacial weathering, including the relative roles of tween distributions. Although we do not directly evaluate temporal sulfide-carbonate vs. silicate mineral weathering compared with variability, dissolved major element concentrations in river waters rivers not dominated by glacial processes. We then consider the vary only slightly over time (38) relative to differences between possible implications for global-scale fluxes in the Quaternary catchments. Dissolved K:Na ratios, which reflect the stoichiometry carbon cycle and for planetary feedbacks over
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