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Title: Uranium isotope fractionation by abiotic reductive precipitation

Abstract

Significant uranium (U) isotope fractionation has been observed during abiotic reduction of aqueous U, counter to the expectation that uranium isotopes are only fractionated by bioassociated enzymatic reduction. In our experiments, aqueous U is removed from solution by reductive precipitation onto the surfaces of synthetic iron monosulfide. The magnitude of uranium isotopic fractionation increases with decreasing aqueous U removal rate and with increasing amounts of neutrally charged aqueous Ca-U-CO 3 species. Here, our discovery means that abiotic U isotope fractionation likely occurs in any reducing environment with aqueous Ca ≥ 1 mM, and that the magnitude of isotopic fractionation changes in response to changes in aqueous major ion concentrations that affect U speciation. Our results have implications for the study of anoxia in the ancient oceans and other environments.

Authors:
ORCiD logo; ; ; ;
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1464871
Alternate Identifier(s):
OSTI ID: 1476603
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 115 Journal Issue: 35; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Country of Publication:
United States
Language:
English
Subject:
07 ISOTOPE AND RADIATION SOURCES; uranium; abiotic fractionation; isotopes; isotope fractionation

Citation Formats

Brown, Shaun T., Basu, Anirban, Ding, Xin, Christensen, John N., and DePaolo, Donald J. Uranium isotope fractionation by abiotic reductive precipitation. United States: N. p., 2018. Web. doi:10.1073/pnas.1805234115.
Brown, Shaun T., Basu, Anirban, Ding, Xin, Christensen, John N., & DePaolo, Donald J. Uranium isotope fractionation by abiotic reductive precipitation. United States. doi:10.1073/pnas.1805234115.
Brown, Shaun T., Basu, Anirban, Ding, Xin, Christensen, John N., and DePaolo, Donald J. Thu . "Uranium isotope fractionation by abiotic reductive precipitation". United States. doi:10.1073/pnas.1805234115.
@article{osti_1464871,
title = {Uranium isotope fractionation by abiotic reductive precipitation},
author = {Brown, Shaun T. and Basu, Anirban and Ding, Xin and Christensen, John N. and DePaolo, Donald J.},
abstractNote = {Significant uranium (U) isotope fractionation has been observed during abiotic reduction of aqueous U, counter to the expectation that uranium isotopes are only fractionated by bioassociated enzymatic reduction. In our experiments, aqueous U is removed from solution by reductive precipitation onto the surfaces of synthetic iron monosulfide. The magnitude of uranium isotopic fractionation increases with decreasing aqueous U removal rate and with increasing amounts of neutrally charged aqueous Ca-U-CO3 species. Here, our discovery means that abiotic U isotope fractionation likely occurs in any reducing environment with aqueous Ca ≥ 1 mM, and that the magnitude of isotopic fractionation changes in response to changes in aqueous major ion concentrations that affect U speciation. Our results have implications for the study of anoxia in the ancient oceans and other environments.},
doi = {10.1073/pnas.1805234115},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 35,
volume = 115,
place = {United States},
year = {2018},
month = {8}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1073/pnas.1805234115

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Cited by: 5 works
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