![Sample our Physical Sciences journals, sign in here to start your FREE access for 14 days]({"type":"image" , "src" : "/sda/110819/TOC-Subject-Sample-2021-Physical-Sciences.jpg"})
Abstract
In this study, the U isotope composition, n(238U)/n(235U), of major components of the upper continental crust, including granitic rocks of different age and post-Archaean shales, as well as that of rivers (the major U source to the oceans) was investigated. Furthermore, U isotope fractionation during the removal of U at mid-ocean ridges, an important sink for U from the oceans, was investigated by the analyses of hydrothermal water samples (including low- and high-temperature fluids), low-temperature altered basalts and calcium carbonate veins. All analysed rock samples from the continental crust fall into a limited range of δ238U between −0.45 and −0.21 ‰ (relative to NBL CRM 112-A), with an average of −0.30 ± 0.15 ‰ (2 SD, N = 11). Despite differences in catchment lithologies, all major rivers define a relatively narrow range between −0.31 and −0.13 ‰, with a weighted mean isotope composition of −0.27 ‰, which is indistinguishable from the estimate for the upper continental crust (−0.30 ‰). Only some tributary rivers from the Swiss Alps display a slightly larger range in δ238U (−0.29 to +0.01 ‰) and lower U concentrations (0.87–3.08 nmol/kg) compared to the investigated major rivers (5.19–11.69 nmol/kg). These findings indicate that only minor net U isotope fractionation occurs during weathering and transport of material from the continental crust to the oceans. Altered basalts display moderately enriched U concentrations (by a factor of 3–18) compared to those typically observed for normal mid-ocean ridge basalts. These, and carbonate veins within altered basalts, show large U isotope fractionation towards both heavy and light U isotope compositions (ranging from −0.63 to +0.27 ‰). Hydrothermal water samples display low U concentrations (0.3–1 nmol/kg) and only limited variations in their U isotope composition (−0.43 ± 0.25 ‰) around the seawater value. Nevertheless, two of the investigated fluids display significantly lower δ238U (−0.55 and −0.59 ‰) than seawater (−0.38 ‰). These findings, together with the heavier U isotope composition observed for some altered basalts and carbonate veins support a model, in which redox processes mostly drive U isotope fractionation. This may result in a slightly heavier U isotope composition of U that is removed from seawater during hydrothermal seafloor alteration compared to that of seawater. Using the estimated isotope compositions of rivers and all U sinks from the ocean (of this study and the literature) for modelling of the isotopic U mass balance, this gives reasonable results for recent estimates of the oceanic U budget. It furthermore provides additional constraints on the relative size of the diverse U sinks and respective net isotope fractionation during U removal.
Acknowledgements
We are grateful to Wolfgang Bach (University of Bremen), Axel Gerdes (University of Frankfurt), Armin Zeh (University of Frankfurt), Elis Hoffmann (University of Bonn) and Carsten Münker (University of Cologne) for providing samples. We thank Anna K. Neumann (University of Frankfurt) and Michael H. Seitz (University of Frankfurt) for laboratory assistance. We thank Morten B. Andersen, Greg A. Brennecka and one anonymous reviewer for their constructive reviews.
Disclosure statement
No potential conflict of interest was reported by the authors.
Supplemental data
Supplemental data for this article can be accessed 10.1080/10256016.2015.1047449.
Notes
1. The original values of [Citation6] were analyzed relative to NIST SRM 950-A, resulting in a shift of +0.04 ‰, compared to our measurements relative to NBL CRM 112-A (see Supplementary text). Here, we report all δ238U values relative to NBL CRM 112-A.