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Title: A XANES and Raman investigation of sulfur speciation and structural order in Murchison and Allende meteorites

Abstract

Abstract Insoluble organic matter ( IOM ) and hydrothermally treated IOM extracted from two carbonaceous chondrites, Murchison and Allende, was studied using sulfur K‐edge XANES (X‐ray absorption near edge structure) and μ‐Raman spectroscopy, with the aim to understand their IOM 's sulfur speciation and structural order, and how aqueous alteration or thermal metamorphism may have transformed these materials. We found that the sulfur‐functional group chemistry of both the Murchison IOM and hydrothermally treated IOM samples have a large chemical variability ranging from oxidation states of S −2 to S +6 , and exhibit a transformation in their oxidation state after the hydrothermal treatment ( HT ) to produce thiophenes and thiol compounds. Sulfoxide and sulfite peaks are also present in Murchison. Sulfates considered intrinsic to Murchison are most likely preaccretionary in nature, and not a result of reactions with water at high temperatures on the asteroid parent body. We argue that the reduced sulfides may have formed in the CM parent body, while the thiophenes and thiol compounds are a result of the HT . Micro‐Raman spectra show the presence of aliphatic and aromatic moieties in Murchison's material as observed previously, which exhibits no change after HT . Because themore » Murchison IOM was modified, as seen by XANES analysis, absence of a change observed using micro‐Raman indicated that although the alkyl carbons of IOM were cleaved, the aromatic network was not largely modified after HT . By contrast, Allende IOM contains primarily disulfide and elemental sulfur, no organic sulfur, and shows no transformation after HT . This nontransformation of Allende IOM after HT would indicate that parent body alteration of sulfide to sulfate is not feasible up to temperatures of 300°C. The reduced sulfur products indicate extreme secondary chemical processing from the precursor compounds in its parent body at temperatures as high as 624°C, as estimated from μ‐Raman D band parameters. The Raman parameters in Allende IOM that was interpreted in terms of amorphous carbon with regions of large clusters of benzene rings, was transformed after the HT to those with fewer benzene rings.« less

Authors:
ORCiD logo [1];  [2];  [1]
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  1. School of Molecular Sciences Arizona State University Tempe Arizona 85283‐1604 USA
  2. Department of Soil, Water &, Environmental Science University of Arizona Tucson Arizona 85721‐0038 USA
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1400613
Resource Type:
Publisher's Accepted Manuscript
Journal Name:
Meteoritics and Planetary Science
Additional Journal Information:
Journal Name: Meteoritics and Planetary Science Journal Volume: 52 Journal Issue: 3; Journal ID: ISSN 1086-9379
Publisher:
Wiley-Blackwell
Country of Publication:
United States
Language:
English

Citation Formats

Bose, M., Root, R. A., and Pizzarello, S. A XANES and Raman investigation of sulfur speciation and structural order in Murchison and Allende meteorites. United States: N. p., 2017. Web. doi:10.1111/maps.12811.
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Bose, M., Root, R. A., & Pizzarello, S. A XANES and Raman investigation of sulfur speciation and structural order in Murchison and Allende meteorites. United States. https://doi.org/10.1111/maps.12811
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Bose, M., Root, R. A., and Pizzarello, S. Thu . "A XANES and Raman investigation of sulfur speciation and structural order in Murchison and Allende meteorites". United States. https://doi.org/10.1111/maps.12811.
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@article{osti_1400613,
title = {A XANES and Raman investigation of sulfur speciation and structural order in Murchison and Allende meteorites},
author = {Bose, M. and Root, R. A. and Pizzarello, S.},
abstractNote = {Abstract Insoluble organic matter ( IOM ) and hydrothermally treated IOM extracted from two carbonaceous chondrites, Murchison and Allende, was studied using sulfur K‐edge XANES (X‐ray absorption near edge structure) and μ‐Raman spectroscopy, with the aim to understand their IOM 's sulfur speciation and structural order, and how aqueous alteration or thermal metamorphism may have transformed these materials. We found that the sulfur‐functional group chemistry of both the Murchison IOM and hydrothermally treated IOM samples have a large chemical variability ranging from oxidation states of S −2 to S +6 , and exhibit a transformation in their oxidation state after the hydrothermal treatment ( HT ) to produce thiophenes and thiol compounds. Sulfoxide and sulfite peaks are also present in Murchison. Sulfates considered intrinsic to Murchison are most likely preaccretionary in nature, and not a result of reactions with water at high temperatures on the asteroid parent body. We argue that the reduced sulfides may have formed in the CM parent body, while the thiophenes and thiol compounds are a result of the HT . Micro‐Raman spectra show the presence of aliphatic and aromatic moieties in Murchison's material as observed previously, which exhibits no change after HT . Because the Murchison IOM was modified, as seen by XANES analysis, absence of a change observed using micro‐Raman indicated that although the alkyl carbons of IOM were cleaved, the aromatic network was not largely modified after HT . By contrast, Allende IOM contains primarily disulfide and elemental sulfur, no organic sulfur, and shows no transformation after HT . This nontransformation of Allende IOM after HT would indicate that parent body alteration of sulfide to sulfate is not feasible up to temperatures of 300°C. The reduced sulfur products indicate extreme secondary chemical processing from the precursor compounds in its parent body at temperatures as high as 624°C, as estimated from μ‐Raman D band parameters. The Raman parameters in Allende IOM that was interpreted in terms of amorphous carbon with regions of large clusters of benzene rings, was transformed after the HT to those with fewer benzene rings.},
doi = {10.1111/maps.12811},
journal = {Meteoritics and Planetary Science},
number = 3,
volume = 52,
place = {United States},
year = {Thu Feb 23 00:00:00 EST 2017},
month = {Thu Feb 23 00:00:00 EST 2017}
}
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https://doi.org/10.1111/maps.12811
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