Diagenetic effects on uranium isotope fractionation in carbonate sediments from the Bahamas

Xinming Chen, Stephen J. Romaniello, Achim D. Herrmann, Dalton Hardisty, Benjamin C. Gill, Ariel Anbar

Research output: Contribution to journalArticle

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Abstract

Uranium isotope variations (δ238U) recorded in sedimentary carbonate rocks are a promising new proxy for the extent of oceanic anoxia through geological time. However, the effects of diagenetic alteration on the U isotopic composition in carbonate sediments, which are crucial to understand the accurate reconstruction of marine δ238U, are currently poorly constrained. Here we examine the effects of the aragonite-to-calcite transition in the Pleistocene Key Largo Limestone of South Florida, and assess the effects of vadose meteoric, phreatic meteoric, and phreatic marine diagenesis on U isotope fractionation in carbonate sediments from the Bahamas Transect, including the well-studied Clino, Unda, and ODP Site 1006 drill cores. Our results suggest that early diagenetic processes in Bahamas carbonate sediments fractionate U isotopes by an average of 0.27 ± 0.14‰ (1 SD) heavier than contemporaneous seawater. Downcore variations of δ238U in slope and basin sediments display little, if any, correlation with U concentration and common geochemical indicators of diagenesis (δ13C, δ18O, Mn/Sr, Mg/Ca, Sr/Ca), enrichments of redox-sensitive elements, or rare earth elements anomalies. We propose two possible mechanisms to interpret the positive change in the δ238U during carbonate diagenesis: authigenic enrichment of isotopically positive U(IV) in carbonates and preferential incorporation of isotopically positive aqueous U(VI) species into carbonates. These processes likely operate during early (syndepositional) diagenesis on the banktop. Further diagenesis during deeper burial is limited by the low solubility of U(IV) under reducing pore water conditions. The early diagenetic behavior of U isotopes in Bahamas carbonate sediments is likely broadly representative of carbonate diagenesis in the geological past. We suggest that the mean diagenetic offset determined in this study be applied when reconstructing seawater δ238U from ancient carbonates. Furthermore, early diagenesis induces significant statistical variability in sediment δ238U values, pointing to the need for large, high resolution data sets in order to average out stochastic variations in individual bulk sediment samples.

Original languageEnglish (US)
Pages (from-to)294-311
Number of pages18
JournalGeochimica et Cosmochimica Acta
Volume237
DOIs
StatePublished - Sep 15 2018

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uranium isotope
Uranium
carbonate sediment
Carbonates
Fractionation
Isotopes
diagenesis
Sediments
fractionation
carbonate
Calcium Carbonate
isotope
sediment
Seawater
seawater
geological time
anoxia
aragonite
effect
Ocean Drilling Program

Keywords

  • Carbonates
  • Diagenesis
  • Paleoredox proxy
  • Uranium isotopes

ASJC Scopus subject areas

  • Geochemistry and Petrology

Cite this

Diagenetic effects on uranium isotope fractionation in carbonate sediments from the Bahamas. / Chen, Xinming; Romaniello, Stephen J.; Herrmann, Achim D.; Hardisty, Dalton; Gill, Benjamin C.; Anbar, Ariel.

In: Geochimica et Cosmochimica Acta, Vol. 237, 15.09.2018, p. 294-311.

Research output: Contribution to journalArticle

Chen, Xinming ; Romaniello, Stephen J. ; Herrmann, Achim D. ; Hardisty, Dalton ; Gill, Benjamin C. ; Anbar, Ariel. / Diagenetic effects on uranium isotope fractionation in carbonate sediments from the Bahamas. In: Geochimica et Cosmochimica Acta. 2018 ; Vol. 237. pp. 294-311.
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AU - Hardisty, Dalton

AU - Gill, Benjamin C.

AU - Anbar, Ariel

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N2 - Uranium isotope variations (δ238U) recorded in sedimentary carbonate rocks are a promising new proxy for the extent of oceanic anoxia through geological time. However, the effects of diagenetic alteration on the U isotopic composition in carbonate sediments, which are crucial to understand the accurate reconstruction of marine δ238U, are currently poorly constrained. Here we examine the effects of the aragonite-to-calcite transition in the Pleistocene Key Largo Limestone of South Florida, and assess the effects of vadose meteoric, phreatic meteoric, and phreatic marine diagenesis on U isotope fractionation in carbonate sediments from the Bahamas Transect, including the well-studied Clino, Unda, and ODP Site 1006 drill cores. Our results suggest that early diagenetic processes in Bahamas carbonate sediments fractionate U isotopes by an average of 0.27 ± 0.14‰ (1 SD) heavier than contemporaneous seawater. Downcore variations of δ238U in slope and basin sediments display little, if any, correlation with U concentration and common geochemical indicators of diagenesis (δ13C, δ18O, Mn/Sr, Mg/Ca, Sr/Ca), enrichments of redox-sensitive elements, or rare earth elements anomalies. We propose two possible mechanisms to interpret the positive change in the δ238U during carbonate diagenesis: authigenic enrichment of isotopically positive U(IV) in carbonates and preferential incorporation of isotopically positive aqueous U(VI) species into carbonates. These processes likely operate during early (syndepositional) diagenesis on the banktop. Further diagenesis during deeper burial is limited by the low solubility of U(IV) under reducing pore water conditions. The early diagenetic behavior of U isotopes in Bahamas carbonate sediments is likely broadly representative of carbonate diagenesis in the geological past. We suggest that the mean diagenetic offset determined in this study be applied when reconstructing seawater δ238U from ancient carbonates. Furthermore, early diagenesis induces significant statistical variability in sediment δ238U values, pointing to the need for large, high resolution data sets in order to average out stochastic variations in individual bulk sediment samples.

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