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Development and Initial Biogeochemical Applications of Compound-Specific Sulfur Isotope Analysis

Greenwood, P. F. and Amrani, A. and Sessions, A. and Raven, M. R. and Holman, A. and Dror, G. and Grice, K. and McCulloch, M. T. and Adkins, J. F. (2014) Development and Initial Biogeochemical Applications of Compound-Specific Sulfur Isotope Analysis. In: Principles and Practice of Analytical Techniques in Geosciences. RSC detection science series. No.4. Royal Society of Chemistry , Cambridge, pp. 285-312. ISBN 978-1-84973-649-7. http://resolver.caltech.edu/CaltechAUTHORS:20160801-104531843

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Abstract

Compound-specific isotope analysis (CSIA) has been extended to the ^(32)S and ^(34)S stable isotopes of sulfur (δ^(34)S) through the combination of gas chromatography (GC) and multi-collector inductively coupled mass spectrometry (ICPMS). The molecular level resolution of sulfur-CSIA is greatly expanding the biogeochemical applications of existing sulfur isotope methods, particularly with respect to organic sulfur compounds. Sulfur participates in a variety of important biogeochemical and redox processes, with distinctive isotopic fractionations accompanying many of these. For example, hydrogen sulfide produced during microbial sulfate reduction can be strongly depleted in ^(34)S (up to 66‰ in δ^(34)S) compared to the source sulfate. An improved understanding of sulfur biogeochemistry at the molecular level will assist in the interpretation of studies of sulfur cycling associated with the modern and paleo-environments. A comparison of δ34S values between organic and inorganic sulfur species may help to illuminate the complex role of sulfur in sedimentary organic diagenesis and the pathways of organic sulfur formation. The δ^(34)S values of individual organic sulfur compounds from natural settings can be currently measured by GC-ICPMS with impressive accuracy, precision (<0.5‰) and sensitivity (≥20 pmol S) over a broad range of analyte volatility. The new sulfur-CSIA capability has already been used to study pathways of early diagenetic organic sulfurisation, volatile sulfur emission from the oceans, oil correlations, thermochemical sulfate reduction of petroleum hydrocarbons, and the relationship between OSCs and mineralising sulfides of large metal deposits.


Item Type:Book Section
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1039/9781782625025-00285DOIArticle
http://pubs.rsc.org/en/Content/Chapter/9781782625025-00285/978-1-78262-502-5PublisherArticle
ORCID:
AuthorORCID
Sessions, A.0000-0001-6120-2763
Additional Information:© 2015 Royal Society of Chemistry. PG, KG, AH, and MM acknowledge funding support from CSIRO Flagship Collaboration Fund Cluster for Organic Geochemistry of Mineral Systems and KG also from an ARC Discovery Outstanding Research Award. AA thanks Shimon Feinstein, Itay Reznik, and IEI Ltd for the oil shale and oil samples from Aderet 1 drillhole and the support of ISF grant 1269/12. ALS and MRR acknowledge the support of NSF EAR-1024919. Our valued instrument technicians, Guillaume Paris (Caltech), Kai Rankenburg (UWA), and Ward Said-Ahmad (HUJI) are thanked for extensive help in developing, maintaining, and implementing the respective sulfur-CSIA systems. Michael Böttcher is thanked for an insightful peer review which helped improve this manuscript.
Funders:
Funding AgencyGrant Number
Commonwealth Scientific and Research Organization (CSIRO)UNSPECIFIED
Australian Research CouncilUNSPECIFIED
Isreal Science Foundation1269/12
NSFEAR-1024919
Record Number:CaltechAUTHORS:20160801-104531843
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20160801-104531843
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:69348
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:01 Aug 2016 18:02
Last Modified:01 Aug 2016 18:05

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