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Micro-scale isotopic variability of low-temperature pyrite in fractured crystalline bedrock ― A large Fe isotope fractionation between Fe(II)aq/pyrite and absence of Fe-S isotope co-variation
Linnaeus University, Faculty of Health and Life Sciences, Department of Biology and Environmental Science.ORCID iD: 0000-0002-0635-3718
Linnaeus University, Faculty of Health and Life Sciences, Department of Biology and Environmental Science.ORCID iD: 0000-0001-7230-6509
Linnaeus University, Faculty of Health and Life Sciences, Department of Biology and Environmental Science. (Ctr Ecol & Evolut Microbial Model Syst EEMiS)ORCID iD: 0000-0003-3588-6676
Swedish Museum of Natural History, Sweden.
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2019 (English)In: Chemical Geology, ISSN 0009-2541, E-ISSN 1872-6836, Vol. 522, p. 192-207Article in journal (Refereed) Published
Abstract [en]

This study assessed Fe-isotope ratio (56Fe/54Fe, expressed as δ56Fe relative to the IRMM-014 standard) variability and controls in pyrite that has among the largest reported S-isotope variability (maximum δ34S: 140‰). The pyrite occurs as fine-grained secondary crystals in fractures throughout the upper kilometer of granitoids of the Baltic Shield, and was analyzed here for δ56Fe by in situ secondary ion mass spectrometry (SIMS). Part of these pyrite crystals were picked from borehole instrumentation at depths of >400 m below sea level (m.b.s.l.), and thus are modern (known to have formed within 17 years) and can be compared with the δ56Fe of the source dissolved ferrous iron. The δ56Fe values of the modern pyrite crystals (−1.81‰ to +2.29‰) varied to a much greater extent than those of the groundwaters from which they formed (−0.48‰ to +0.13‰), providing strong field evidence for a large Fe isotope fractionation during the conversion of Fe(II)aq to FeS and ultimately to pyrite. Enrichment of 56Fe in pyrite relative to the groundwater was explained by equilibrium Fe(II)aq-FeS isotope fractionation, whereas depletion of 56Fe in pyrite relative to the groundwater was mainly the result of sulfidization of magnetite and kinetic isotopic fractionation during partial transformation of microsized FeS to pyrite. In many pyrite crystals, there is an increase in δ34S from crystal center to rim reflecting Rayleigh distillation processes (reservoir effects) caused by the development of closed-system conditions in the micro-environment near the growing crystals. A corresponding center-to-rim feature was not observed for the δ56Fe values. It is therefore unlikely that the groundwater near the growing pyrite crystals became progressively enriched in the heavy Fe isotope, in contrast to what has been found for the sulfur in sulfate. Other pyrite crystals formed following bacterial sulfate reduction in the time period of mid-Mesozoicum to Quaternary, had an almost identical Fe-isotope variability (total range: −1.50‰ to +2.76‰), frequency-distribution pattern, and relationship with δ34S as the recent pyrite formed on the borehole instrumentation. These features suggest that fundamental processes are operating and governing the Fe-isotope composition of pyrite crystals formed in fractured crystalline bedrock over large time scales.

Place, publisher, year, edition, pages
Elsevier, 2019. Vol. 522, p. 192-207
Keywords [en]
Pyrite, Iron isotopes, Equilibrium Fe-isotope fractionation, Magnetite sulfidization, Partial pyritization, Fractured crystalline bedrock
National Category
Earth and Related Environmental Sciences
Research subject
Natural Science, Environmental Science
Identifiers
URN: urn:nbn:se:lnu:diva-84618DOI: 10.1016/j.chemgeo.2019.05.026ISI: 000480330600016Scopus ID: 2-s2.0-85066994013OAI: oai:DiVA.org:lnu-84618DiVA, id: diva2:1320554
Funder
Swedish Research Council, 2017-05186Swedish Research Council, 2014-4398Swedish Research Council Formas, 2017-00766Available from: 2019-06-05 Created: 2019-06-05 Last updated: 2019-08-29Bibliographically approved

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Yu, ChangxunDrake, HenrikLopez-Fernandez, MargaritaDopson, MarkÅström, Mats E.

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