Sulfur isotope fractionation between aqueous and carbonate-associated sulfate in abiotic calcite and aragonite

Barkan, Yigal; Paris, Guillaume; Webb, Samuel M.; Adkins, Jess F.; Halevy, Itay

doi:10.1016/j.gca.2020.03.022

Sulfur isotope fractionation between aqueous and carbonate-associated sulfate in abiotic calcite and aragonite

Journal Article · Tue Mar 24 00:00:00 EDT 2020 · Geochimica et Cosmochimica Acta

DOI:https://doi.org/10.1016/j.gca.2020.03.022· OSTI ID:1637646

^[1]; ^[2]; Webb, Samuel M. ^[3]; Adkins, Jess F. ^[4]; Halevy, Itay ^[1]

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)

Sulfate (SO₄^2–) 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-SO₄^2– isotope fractionation) on sulfate concentration and precipitation rate. In aragonite, the CAS-SO₄^2– isotope fractionation is 1.0 ± 0.3‰ and independent of the sulfate (and CAS) concentration. In contrast, we note the CAS-SO₄^2– 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-SO₄^2– 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.

View Accepted Manuscript (DOE)

Research Organization:: SLAC National Accelerator Laboratory, Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)

Sponsoring Organization:: European Research Council (ERC); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1637646

Alternate ID(s):: OSTI ID: 1775796

Journal Information:: Geochimica et Cosmochimica Acta, Journal Name: Geochimica et Cosmochimica Acta Journal Issue: C Vol. 280; ISSN 0016-7037

Publisher:: Elsevier; The Geochemical Society; The Meteoritical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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