Reductive defluorination of perfluorooctane sulfonate

Valeria Ochoa-Herrera; Reyes Sierra-Alvarez; Arpad Somogyi; Neil E. Jacobsen; Vicki H. Wysocki; Jim A. Field

doi:10.1021/es702842q

Reductive defluorination of perfluorooctane sulfonate

Valeria Ochoa-Herrera
, Reyes Sierra-Alvarez^*
, Arpad Somogyi
, Neil E. Jacobsen
, Vicki H. Wysocki
, Jim A. Field

^*Corresponding author for this work

University of Arizona
Department of Chemistry and Biochemistry

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

135 Scopus citations

Abstract

Perfluorooctane sulfonate (PFOS) is under increased scrutiny as an environmental pollutant due to recent reports of its worldwide distribution, environmental persistence, and bioaccumulation potential. The susceptibility of technical PFOS and PFOS branched isomers to chemical reductive dehalogenation with vitamin B ₁₂ (260 μ.M) as catalyst and Ti(lll)-citrate (36 mM) as bulk reductant in anoxic aqueous solution at 70 °C and pH 9 was evaluated in this study. Defluorination was confirmed by fluoride release measurements of 18% in technical PFOS, equivalent to the removal 3 mol F ^-/mol PFOS, and 71% in PFOS branched isomers equivalent to the removal of 12 mol F ^-/mol PFOS. Degradation of PFOS was further confirmed by monitoring the disappearance of PFOS compounds with reaction time by suppressed conductivity ion chromatography, LC-MS/MS, and ¹⁹F NMR studies. The PFOS compounds differed in their susceptibility to reductive degradation by vitamin B ₁₂/Ti(lll) citrate. Chromatographic peaks corresponding to branched PFOS isomers disappeared whereas the peak corresponding to linear PFOS was stable. To our knowledge this is the first report of reductive dehalogenation of PFOS catalyzed by a biomolecule.

Original language	English
Pages (from-to)	3260-3264
Number of pages	5
Journal	Environmental Science and Technology
Volume	42
Issue number	9
DOIs	https://doi.org/10.1021/es702842q
State	Published - 1 May 2008
Externally published	Yes

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10.1021/es702842q

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title = "Reductive defluorination of perfluorooctane sulfonate",

abstract = "Perfluorooctane sulfonate (PFOS) is under increased scrutiny as an environmental pollutant due to recent reports of its worldwide distribution, environmental persistence, and bioaccumulation potential. The susceptibility of technical PFOS and PFOS branched isomers to chemical reductive dehalogenation with vitamin B 12 (260 μ.M) as catalyst and Ti(lll)-citrate (36 mM) as bulk reductant in anoxic aqueous solution at 70 °C and pH 9 was evaluated in this study. Defluorination was confirmed by fluoride release measurements of 18\% in technical PFOS, equivalent to the removal 3 mol F -/mol PFOS, and 71\% in PFOS branched isomers equivalent to the removal of 12 mol F -/mol PFOS. Degradation of PFOS was further confirmed by monitoring the disappearance of PFOS compounds with reaction time by suppressed conductivity ion chromatography, LC-MS/MS, and 19F NMR studies. The PFOS compounds differed in their susceptibility to reductive degradation by vitamin B 12/Ti(lll) citrate. Chromatographic peaks corresponding to branched PFOS isomers disappeared whereas the peak corresponding to linear PFOS was stable. To our knowledge this is the first report of reductive dehalogenation of PFOS catalyzed by a biomolecule.",

author = "Valeria Ochoa-Herrera and Reyes Sierra-Alvarez and Arpad Somogyi and Jacobsen, \{Neil E.\} and Wysocki, \{Vicki H.\} and Field, \{Jim A.\}",

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T1 - Reductive defluorination of perfluorooctane sulfonate

AU - Ochoa-Herrera, Valeria

AU - Sierra-Alvarez, Reyes

AU - Somogyi, Arpad

AU - Jacobsen, Neil E.

AU - Wysocki, Vicki H.

AU - Field, Jim A.

PY - 2008/5/1

Y1 - 2008/5/1

N2 - Perfluorooctane sulfonate (PFOS) is under increased scrutiny as an environmental pollutant due to recent reports of its worldwide distribution, environmental persistence, and bioaccumulation potential. The susceptibility of technical PFOS and PFOS branched isomers to chemical reductive dehalogenation with vitamin B 12 (260 μ.M) as catalyst and Ti(lll)-citrate (36 mM) as bulk reductant in anoxic aqueous solution at 70 °C and pH 9 was evaluated in this study. Defluorination was confirmed by fluoride release measurements of 18% in technical PFOS, equivalent to the removal 3 mol F -/mol PFOS, and 71% in PFOS branched isomers equivalent to the removal of 12 mol F -/mol PFOS. Degradation of PFOS was further confirmed by monitoring the disappearance of PFOS compounds with reaction time by suppressed conductivity ion chromatography, LC-MS/MS, and 19F NMR studies. The PFOS compounds differed in their susceptibility to reductive degradation by vitamin B 12/Ti(lll) citrate. Chromatographic peaks corresponding to branched PFOS isomers disappeared whereas the peak corresponding to linear PFOS was stable. To our knowledge this is the first report of reductive dehalogenation of PFOS catalyzed by a biomolecule.

AB - Perfluorooctane sulfonate (PFOS) is under increased scrutiny as an environmental pollutant due to recent reports of its worldwide distribution, environmental persistence, and bioaccumulation potential. The susceptibility of technical PFOS and PFOS branched isomers to chemical reductive dehalogenation with vitamin B 12 (260 μ.M) as catalyst and Ti(lll)-citrate (36 mM) as bulk reductant in anoxic aqueous solution at 70 °C and pH 9 was evaluated in this study. Defluorination was confirmed by fluoride release measurements of 18% in technical PFOS, equivalent to the removal 3 mol F -/mol PFOS, and 71% in PFOS branched isomers equivalent to the removal of 12 mol F -/mol PFOS. Degradation of PFOS was further confirmed by monitoring the disappearance of PFOS compounds with reaction time by suppressed conductivity ion chromatography, LC-MS/MS, and 19F NMR studies. The PFOS compounds differed in their susceptibility to reductive degradation by vitamin B 12/Ti(lll) citrate. Chromatographic peaks corresponding to branched PFOS isomers disappeared whereas the peak corresponding to linear PFOS was stable. To our knowledge this is the first report of reductive dehalogenation of PFOS catalyzed by a biomolecule.

UR - https://www.scopus.com/pages/publications/50649102317

U2 - 10.1021/es702842q

DO - 10.1021/es702842q

M3 - Artículo

C2 - 18522103

AN - SCOPUS:50649102317

SN - 0013-936X

VL - 42

SP - 3260

EP - 3264

JO - Environmental Science and Technology

JF - Environmental Science and Technology

IS - 9

ER -

Reductive defluorination of perfluorooctane sulfonate

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