Evidence of magnetic isotope effects during thermochemical sulfate reduction

Harry Daniel Oduro; Brian Harms; Herman O. Sintim; Alan J. Kaufman; George Cody; James Farquhar

doi:10.1073/pnas.1108112108

Evidence of magnetic isotope effects during thermochemical sulfate reduction

Harry Daniel Oduro, Brian Harms, Herman O. Sintim, Alan J. Kaufman, George Cody, James Farquhar

Research output: Contribution to journal › Article › peer-review

Abstract

Thermochemical sulfate reduction experiments with simple amino acid and dilute concentrations of sulfate reveal significant degrees of mass-independent sulfur isotope fractionation. Enrichments of up to 13% for (33)S are attributed to a magnetic isotope effect (MIE) associated with the formation of thiol-disulfide, ion-radical pairs. Observed (36)S depletions in products are explained here by classical (mass-dependent) isotope effects and mixing processes. The experimental data contrasts strongly with multiple sulfur isotope trends in Archean samples, which exhibit significant (36)S anomalies. These results support an origin other than thermochemical sulfate reduction for the mass-independent signals observed for early Earth samples.

Original language	English
Pages (from-to)	17635-17638
Number of pages	4
Journal	Proceedings of the National Academy of Sciences of the United States of America
Volume	108
Issue number	43
DOIs	https://doi.org/10.1073/pnas.1108112108
Publication status	Published - 25 Oct 2011

Keywords

anomalous
sulfur radical
thermolysis
spin-selective
hyperfine coupling
MASS-INDEPENDENT FRACTIONATION
MULTIPLE SULFUR ISOTOPES
HYDROGEN-SULFIDE
THERMAL-DECOMPOSITION
ARCHEAN ATMOSPHERE
CHEMICAL-REACTIONS
NUCLEAR-SPIN
RADICALS
CARBON
ACIDS

Access to Document

10.1073/pnas.1108112108

Cite this

@article{e01433c8c3c14fa982cda54643a593a4,

title = "Evidence of magnetic isotope effects during thermochemical sulfate reduction",

abstract = "Thermochemical sulfate reduction experiments with simple amino acid and dilute concentrations of sulfate reveal significant degrees of mass-independent sulfur isotope fractionation. Enrichments of up to 13% for (33)S are attributed to a magnetic isotope effect (MIE) associated with the formation of thiol-disulfide, ion-radical pairs. Observed (36)S depletions in products are explained here by classical (mass-dependent) isotope effects and mixing processes. The experimental data contrasts strongly with multiple sulfur isotope trends in Archean samples, which exhibit significant (36)S anomalies. These results support an origin other than thermochemical sulfate reduction for the mass-independent signals observed for early Earth samples.",

keywords = "anomalous, sulfur radical, thermolysis, spin-selective, hyperfine coupling, MASS-INDEPENDENT FRACTIONATION, MULTIPLE SULFUR ISOTOPES, HYDROGEN-SULFIDE, THERMAL-DECOMPOSITION, ARCHEAN ATMOSPHERE, CHEMICAL-REACTIONS, NUCLEAR-SPIN, RADICALS, CARBON, ACIDS",

author = "Oduro, {Harry Daniel} and Brian Harms and Sintim, {Herman O.} and Kaufman, {Alan J.} and George Cody and James Farquhar",

year = "2011",

month = oct,

day = "25",

doi = "10.1073/pnas.1108112108",

language = "English",

volume = "108",

pages = "17635--17638",

journal = "Proceedings of the National Academy of Sciences of the United States of America",

issn = "0027-8424",

publisher = "NATL ACAD SCIENCES",

number = "43",

}

TY - JOUR

T1 - Evidence of magnetic isotope effects during thermochemical sulfate reduction

AU - Oduro, Harry Daniel

AU - Harms, Brian

AU - Sintim, Herman O.

AU - Kaufman, Alan J.

AU - Cody, George

AU - Farquhar, James

PY - 2011/10/25

Y1 - 2011/10/25

N2 - Thermochemical sulfate reduction experiments with simple amino acid and dilute concentrations of sulfate reveal significant degrees of mass-independent sulfur isotope fractionation. Enrichments of up to 13% for (33)S are attributed to a magnetic isotope effect (MIE) associated with the formation of thiol-disulfide, ion-radical pairs. Observed (36)S depletions in products are explained here by classical (mass-dependent) isotope effects and mixing processes. The experimental data contrasts strongly with multiple sulfur isotope trends in Archean samples, which exhibit significant (36)S anomalies. These results support an origin other than thermochemical sulfate reduction for the mass-independent signals observed for early Earth samples.

AB - Thermochemical sulfate reduction experiments with simple amino acid and dilute concentrations of sulfate reveal significant degrees of mass-independent sulfur isotope fractionation. Enrichments of up to 13% for (33)S are attributed to a magnetic isotope effect (MIE) associated with the formation of thiol-disulfide, ion-radical pairs. Observed (36)S depletions in products are explained here by classical (mass-dependent) isotope effects and mixing processes. The experimental data contrasts strongly with multiple sulfur isotope trends in Archean samples, which exhibit significant (36)S anomalies. These results support an origin other than thermochemical sulfate reduction for the mass-independent signals observed for early Earth samples.

KW - anomalous

KW - sulfur radical

KW - thermolysis

KW - spin-selective

KW - hyperfine coupling

KW - MASS-INDEPENDENT FRACTIONATION

KW - MULTIPLE SULFUR ISOTOPES

KW - HYDROGEN-SULFIDE

KW - THERMAL-DECOMPOSITION

KW - ARCHEAN ATMOSPHERE

KW - CHEMICAL-REACTIONS

KW - NUCLEAR-SPIN

KW - RADICALS

KW - CARBON

KW - ACIDS

U2 - 10.1073/pnas.1108112108

DO - 10.1073/pnas.1108112108

M3 - Article

SN - 0027-8424

VL - 108

SP - 17635

EP - 17638

JO - Proceedings of the National Academy of Sciences of the United States of America

JF - Proceedings of the National Academy of Sciences of the United States of America

IS - 43

ER -

Evidence of magnetic isotope effects during thermochemical sulfate reduction

Abstract

Keywords

Access to Document

Fingerprint

Cite this