Sulfur isotope fractionation between aqueous and carbonate-associated sulfate in abiotic calcite and aragonite
Abstract
Sulfate (SO42–) incorporated into calcium carbonate minerals enables measurements of sulfur (S) isotope ratios in carbonate rocks. This Carbonate Associated Sulfate (CAS) in marine carbonate minerals is thought to faithfully represent the S isotope composition of the seawater sulfate incorporated into the mineral, with little or no S isotope fractionation in the process. However, comparison between different calcifying species reveals both positive and negative S isotope fractionation between CAS and seawater sulfate, and a large range of S isotope ratios can be found within a single rock sample, depending on the component measured. To better understand the isotopic effects associated with sulfate incorporation into carbonate minerals, we precipitated inorganic calcite and aragonite over a range covering more than two orders of magnitude of sulfate concentration and precipitation rate. Coupled measurements of CAS concentration, S isotope composition and X-ray absorption near-edge spectra (XANES) permit characterization and explanation of the observed dependence of S isotope fractionation between CAS and aqueous sulfate (CAS-SO42– isotope fractionation) on sulfate concentration and precipitation rate. In aragonite, the CAS-SO42– isotope fractionation is 1.0 ± 0.3‰ and independent of the sulfate (and CAS) concentration. In contrast, we note the CAS-SO42– isotope fractionation in calcite covaries strongly with themore »
- Authors:
-
[1];
[2];
- Weizmann Inst. of Science, Rehovot (Israel)
- California Inst. of Technology (CalTech), Pasadena, CA (United States); Univ. de Lorraine (France)
- SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
- California Inst. of Technology (CalTech)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
- Sponsoring Org.:
- European Research Council (ERC); USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1637646
- Alternate Identifier(s):
- OSTI ID: 1775796
- Grant/Contract Number:
- AC02-76SF00515; 337183
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Geochimica et Cosmochimica Acta
- Additional Journal Information:
- Journal Volume: 280; Journal Issue: C; Journal ID: ISSN 0016-7037
- Publisher:
- Elsevier; The Geochemical Society; The Meteoritical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 58 GEOSCIENCES; Sulfur cycle; Partition coefficient; Ion substitution; Sulfur XANES; Experimental mineral precipitation
Citation Formats
Barkan, Yigal, Paris, Guillaume, Webb, Samuel M., Adkins, Jess F., and Halevy, Itay. Sulfur isotope fractionation between aqueous and carbonate-associated sulfate in abiotic calcite and aragonite. United States: N. p., 2020.
Web. doi:10.1016/j.gca.2020.03.022.
Barkan, Yigal, Paris, Guillaume, Webb, Samuel M., Adkins, Jess F., & Halevy, Itay. Sulfur isotope fractionation between aqueous and carbonate-associated sulfate in abiotic calcite and aragonite. United States. https://doi.org/10.1016/j.gca.2020.03.022
Barkan, Yigal, Paris, Guillaume, Webb, Samuel M., Adkins, Jess F., and Halevy, Itay. Tue .
"Sulfur isotope fractionation between aqueous and carbonate-associated sulfate in abiotic calcite and aragonite". United States. https://doi.org/10.1016/j.gca.2020.03.022. https://www.osti.gov/servlets/purl/1637646.
@article{osti_1637646,
title = {Sulfur isotope fractionation between aqueous and carbonate-associated sulfate in abiotic calcite and aragonite},
author = {Barkan, Yigal and Paris, Guillaume and Webb, Samuel M. and Adkins, Jess F. and Halevy, Itay},
abstractNote = {Sulfate (SO42–) incorporated into calcium carbonate minerals enables measurements of sulfur (S) isotope ratios in carbonate rocks. This Carbonate Associated Sulfate (CAS) in marine carbonate minerals is thought to faithfully represent the S isotope composition of the seawater sulfate incorporated into the mineral, with little or no S isotope fractionation in the process. However, comparison between different calcifying species reveals both positive and negative S isotope fractionation between CAS and seawater sulfate, and a large range of S isotope ratios can be found within a single rock sample, depending on the component measured. To better understand the isotopic effects associated with sulfate incorporation into carbonate minerals, we precipitated inorganic calcite and aragonite over a range covering more than two orders of magnitude of sulfate concentration and precipitation rate. Coupled measurements of CAS concentration, S isotope composition and X-ray absorption near-edge spectra (XANES) permit characterization and explanation of the observed dependence of S isotope fractionation between CAS and aqueous sulfate (CAS-SO42– isotope fractionation) on sulfate concentration and precipitation rate. In aragonite, the CAS-SO42– isotope fractionation is 1.0 ± 0.3‰ and independent of the sulfate (and CAS) concentration. In contrast, we note the CAS-SO42– isotope fractionation in calcite covaries strongly with the sulfate concentration and weakly with the precipitation rate, between values of 1.3 ± 0.1 and 3.1 ± 0.6‰. We suggest that the correlation between aqueous sulfate concentration and CAS-SO42– isotope fractionation in calcite reflects a dependence of the equilibrium S isotope fractionation on the concentration of CAS, through the effect of the sulfate impurity on the carbonate mineral’s energetic state.},
doi = {10.1016/j.gca.2020.03.022},
journal = {Geochimica et Cosmochimica Acta},
number = C,
volume = 280,
place = {United States},
year = {Tue Mar 24 00:00:00 EDT 2020},
month = {Tue Mar 24 00:00:00 EDT 2020}
}
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