All data is included within the tables in the paper and supplement.
Uranium isotopes as tracers of serpentinite weathering
Abstract
The aqueous alteration of mantle rocks is considered to play a key role in Earth's global biogeochemical cycling. Uranium enrichment in fluid-altered mantle rocks is a common feature that may reflect redox state or fluid source, but it remains unclear when, why, and how uranium is mobilized within these systems. In this study we use uranium (U) isotopes (234U/238U and 238U/235U ratios) to deduce the timing, mobilization processes, and fluid sources responsible for weathering of subaerial and submarine serpentinites. We find that complex post-formation weathering processes continue to perturb serpentinite U isotope compositions and U concentrations long after initial serpentinization. Enriched 234U/238U ratios in dredged seafloor serpentinites require recent (<1.5 Myr) uptake of U, likely from derived from chemically evolved seawater that has circulated through igneous basement rocks. In contrast, depleted and variable 234U/238U ratios in a terrestrial serpentinite across <30 cm spatial scales from the Wadi Fins outcrop in the Samail Ophiolite, Oman, indicate alpha recoil effects, with differences in these ratios reflecting different grain sizes or shapes of U-hosting minerals in different weathering zones. Both seafloor and Wadi Fins serpentinites have 238U/235U ratios significantly different from seawater and mid-ocean ridge basalts, reflecting different initial protolith composition and/or overprinting of 238U/235U ratios during weathering. Using 238U/235U and U concentrations we calculate the isotopic composition of evolved fluids weathering the serpentinites at both localities. We also use 234U/238U and models of alpha recoil to determine the grain sizes of minerals hosting U from samples at Wadi Fins. Our results suggest that U isotopic compositions and concentrations are sensitive to post-serpentinization weathering processes in subaerial and submarine environments. The U isotopic composition of abyssal serpentinites is set by seawater that has chemically evolved during flow through basement rocks, questioning the utility of weathered serpentinites as an archive of paleo-seawater U isotope compositions, as well as other fluid-mobile elements modified during crustal fluid flow.
Copyright and License (English)
© 2023 Elsevier.
Acknowledgement (English)
F.J.P. was supported by a Stanback Postdoctoral Fellowship at Caltech. EHGC was supported by U.S. National Science Foundation (NSF) grants EAR-1949148 and OCE-2049940 and start-up funds from USC. FLHT is grateful for support from NSF grants EAR-1824002 and MGG-2054892, a Packard Fellowship, a research award from the Heritage Medical Research Institute, and start-up funds provided by Caltech. F.K. was supported by the Independent Research & Development Program “Chemical Weathering of the Oceanic Mantle by Seawater” at WHOI. KWWS acknowledges support from NSF-OCE-1634669. We thank Will Berelson and Nick Rollins at University of Southern California for facilitating the carbonate content measurements. The comments of two anonymous reviewers, as well as the associate editor Laurence Coogan, greatly improved the manuscript.
Contributions (English)
Frank J. Pavia: Methodology, Formal analysis, Investigation, Conceptualization, Writing – original draft, Writing – review & editing. Emily H.G. Cooperdock: Writing – original draft, Writing – review & editing, Conceptualization, Resources. Juan Carlos de Obeso: Writing – original draft, Writing – review & editing, Conceptualization, Resources. Kenneth W.W. Sims: Writing – review & editing. François L.H. Tissot: Resources, Writing – review & editing. Frieder Klein: Resources, Writing – review & editing.
Data Availability (English)
Conflict of Interest (English)
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
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Additional details
- California Institute of Technology
- Foster and Coco Stanback Postdoctoral Fellowship
- National Science Foundation
- EAR-1949148
- National Science Foundation
- OCE-2049940
- University of Southern California
- National Science Foundation
- EAR-1824002
- National Science Foundation
- OCE-2054892
- David and Lucile Packard Foundation
- California Institute of Technology
- Heritage Medical Research Institute
- Woods Hole Oceanographic Institution
- National Science Foundation
- OCE-1634669
- Caltech groups
- Division of Geological and Planetary Sciences, Heritage Medical Research Institute