Details
| Original language | English |
|---|---|
| Pages (from-to) | 345-359 |
| Number of pages | 15 |
| Journal | Geochimica et cosmochimica acta |
| Volume | 72 |
| Issue number | 2 |
| Publication status | Published - 15 Jan 2008 |
| Externally published | Yes |
Abstract
The isotopic composition of U in nature is generally assumed to be invariant. Here, we report variations of the 238U/235U isotope ratio in natural samples (basalts, granites, seawater, corals, black shales, suboxic sediments, ferromanganese crusts/nodules and BIFs) of ∼1.3‰, exceeding by far the analytical precision of our method (≈0.06‰, 2SD). U isotopes were analyzed with MC-ICP-MS using a mixed 236U-233U isotopic tracer (double spike) to correct for isotope fractionation during sample purification and instrumental mass bias. The largest isotope variations found in our survey are between oxidized and reduced depositional environments, with seawater and suboxic sediments falling in between. Light U isotope compositions (relative to SRM-950a) were observed for manganese crusts from the Atlantic and Pacific oceans, which display δ238U of -0.54‰ to -0.62‰ and for three of four analyzed Banded Iron Formations, which have δ238U of -0.89‰, -0.72‰ and -0.70‰, respectively. High δ238U values are observed for black shales from the Black Sea (unit-I and unit-II) and three Kupferschiefer samples (Germany), which display δ238U of -0.06‰ to +0.43‰. Also, suboxic sediments have slightly elevated δ238U (-0.41‰ to -0.16‰) compared to seawater, which has δ238U of -0.41 ± 0.03‰. Granites define a range of δ238U between -0.20‰ and -0.46‰, but all analyzed basalts are identical within uncertainties and slightly lighter than seawater (δ238U = -0.29‰). Our findings imply that U isotope fractionation occurs in both oxic (manganese crusts) and suboxic to euxinic environments with opposite directions. In the first case, we hypothesize that this fractionation results from adsorption of U to ferromanganese oxides, as is the case for Mo and possibly Tl isotopes. In the second case, reduction of soluble UVI to insoluble UIV probably results in fractionation toward heavy U isotope compositions relative to seawater. These findings imply that variable ocean redox conditions through geological time should result in variations of the seawater U isotope compositions, which may be recorded in sediments or fossils. Thus, U isotopes might be a promising novel geochemical tracer for paleo-redox conditions and the redox evolution on Earth. The discovery that 238U/235U varies in nature also has implications for the precision and accuracy of U-Pb dating. The total observed range in U isotope compositions would produce variations in 207Pb/206Pb ages of young U-bearing minerals of up to 3 Ma, and up to 2 Ma for minerals that are 3 billion years old.
ASJC Scopus subject areas
- Earth and Planetary Sciences(all)
- Geochemistry and Petrology
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In: Geochimica et cosmochimica acta, Vol. 72, No. 2, 15.01.2008, p. 345-359.
Research output: Contribution to journal › Article › Research › peer review
}
TY - JOUR
T1 - Natural fractionation of 238U/235U
AU - Weyer, S.
AU - Anbar, A. D.
AU - Gerdes, A.
AU - Gordon, G. W.
AU - Algeo, T. J.
AU - Boyle, E. A.
N1 - Funding information: We thank G. Ravizza for providing Black Sea black shales, Wilhelm Püttmann and Soodabeh Durali-Müller for providing Kupferschiefer samples, Eberhardt Gischler for providing coral samples, the Senckenberg Museum in Frankfurt for providing a manganese nodule and Ulf Linnemann, Alan Woodland and Alexander Schmidt for providing samples from banded iron formations. Gail Arnold and Klaus Mezger are thanked for helpful discussion and Anna Neumann for laboratory assistance. We thank Gideon Henderson, Claudine Stirling and an anonymous reviewer for their constructive reviews. Jim McManus is thanked for editorial handling. This work was supported by grants from the US National Science Foundation (Geobiology & Low Temperature Geochemistry and Instrumentation & Facilities programs) and NASA (Exobiology program) to A.D.A.
PY - 2008/1/15
Y1 - 2008/1/15
N2 - The isotopic composition of U in nature is generally assumed to be invariant. Here, we report variations of the 238U/235U isotope ratio in natural samples (basalts, granites, seawater, corals, black shales, suboxic sediments, ferromanganese crusts/nodules and BIFs) of ∼1.3‰, exceeding by far the analytical precision of our method (≈0.06‰, 2SD). U isotopes were analyzed with MC-ICP-MS using a mixed 236U-233U isotopic tracer (double spike) to correct for isotope fractionation during sample purification and instrumental mass bias. The largest isotope variations found in our survey are between oxidized and reduced depositional environments, with seawater and suboxic sediments falling in between. Light U isotope compositions (relative to SRM-950a) were observed for manganese crusts from the Atlantic and Pacific oceans, which display δ238U of -0.54‰ to -0.62‰ and for three of four analyzed Banded Iron Formations, which have δ238U of -0.89‰, -0.72‰ and -0.70‰, respectively. High δ238U values are observed for black shales from the Black Sea (unit-I and unit-II) and three Kupferschiefer samples (Germany), which display δ238U of -0.06‰ to +0.43‰. Also, suboxic sediments have slightly elevated δ238U (-0.41‰ to -0.16‰) compared to seawater, which has δ238U of -0.41 ± 0.03‰. Granites define a range of δ238U between -0.20‰ and -0.46‰, but all analyzed basalts are identical within uncertainties and slightly lighter than seawater (δ238U = -0.29‰). Our findings imply that U isotope fractionation occurs in both oxic (manganese crusts) and suboxic to euxinic environments with opposite directions. In the first case, we hypothesize that this fractionation results from adsorption of U to ferromanganese oxides, as is the case for Mo and possibly Tl isotopes. In the second case, reduction of soluble UVI to insoluble UIV probably results in fractionation toward heavy U isotope compositions relative to seawater. These findings imply that variable ocean redox conditions through geological time should result in variations of the seawater U isotope compositions, which may be recorded in sediments or fossils. Thus, U isotopes might be a promising novel geochemical tracer for paleo-redox conditions and the redox evolution on Earth. The discovery that 238U/235U varies in nature also has implications for the precision and accuracy of U-Pb dating. The total observed range in U isotope compositions would produce variations in 207Pb/206Pb ages of young U-bearing minerals of up to 3 Ma, and up to 2 Ma for minerals that are 3 billion years old.
AB - The isotopic composition of U in nature is generally assumed to be invariant. Here, we report variations of the 238U/235U isotope ratio in natural samples (basalts, granites, seawater, corals, black shales, suboxic sediments, ferromanganese crusts/nodules and BIFs) of ∼1.3‰, exceeding by far the analytical precision of our method (≈0.06‰, 2SD). U isotopes were analyzed with MC-ICP-MS using a mixed 236U-233U isotopic tracer (double spike) to correct for isotope fractionation during sample purification and instrumental mass bias. The largest isotope variations found in our survey are between oxidized and reduced depositional environments, with seawater and suboxic sediments falling in between. Light U isotope compositions (relative to SRM-950a) were observed for manganese crusts from the Atlantic and Pacific oceans, which display δ238U of -0.54‰ to -0.62‰ and for three of four analyzed Banded Iron Formations, which have δ238U of -0.89‰, -0.72‰ and -0.70‰, respectively. High δ238U values are observed for black shales from the Black Sea (unit-I and unit-II) and three Kupferschiefer samples (Germany), which display δ238U of -0.06‰ to +0.43‰. Also, suboxic sediments have slightly elevated δ238U (-0.41‰ to -0.16‰) compared to seawater, which has δ238U of -0.41 ± 0.03‰. Granites define a range of δ238U between -0.20‰ and -0.46‰, but all analyzed basalts are identical within uncertainties and slightly lighter than seawater (δ238U = -0.29‰). Our findings imply that U isotope fractionation occurs in both oxic (manganese crusts) and suboxic to euxinic environments with opposite directions. In the first case, we hypothesize that this fractionation results from adsorption of U to ferromanganese oxides, as is the case for Mo and possibly Tl isotopes. In the second case, reduction of soluble UVI to insoluble UIV probably results in fractionation toward heavy U isotope compositions relative to seawater. These findings imply that variable ocean redox conditions through geological time should result in variations of the seawater U isotope compositions, which may be recorded in sediments or fossils. Thus, U isotopes might be a promising novel geochemical tracer for paleo-redox conditions and the redox evolution on Earth. The discovery that 238U/235U varies in nature also has implications for the precision and accuracy of U-Pb dating. The total observed range in U isotope compositions would produce variations in 207Pb/206Pb ages of young U-bearing minerals of up to 3 Ma, and up to 2 Ma for minerals that are 3 billion years old.
UR - http://www.scopus.com/inward/record.url?scp=37549046414&partnerID=8YFLogxK
U2 - 10.1016/j.gca.2007.11.012
DO - 10.1016/j.gca.2007.11.012
M3 - Article
AN - SCOPUS:37549046414
VL - 72
SP - 345
EP - 359
JO - Geochimica et cosmochimica acta
JF - Geochimica et cosmochimica acta
SN - 0016-7037
IS - 2
ER -