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Alternate Reductants with VB12 to Transform C8 and C6 Perfluoroalkyl Sulfonates: Limitations and Insights into Isomer-Specific Transformation Rates, Products and Pathways

Park, Saerom, de Perre, Chloe, Lee, Linda S.·2017·Environmental Science & Technology
DOI 10.1021/acs.est.7b03744
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Abstract

Previous studies evaluating Vitamin B12 (VB12) with Ti(III)-citrate for potential use in in situ remediation of perfluorooctanesulfonate (PFOS) found that linear (L)-PFOS was unaltered. We explored if alternate reductants could overcome this limitation with a primary focus on nanoscale zerovalent zinc (nZn 0 ). Transformation over time with VB12-nZn 0 was quantified at 22, 70, and 90 °C for PFOS, at 70 °C for perfluorohexanesulfonate (PFHxS), and VB12-nFe 0 and VB12-Pd 0 /nFe 0 at 70 °C for PFOS. Only branched (br-) isomers were transformed generating F - (no SO 4 2- ) and polyfluoroalkyl intermediates/products. The absence of L-PFOS transformation by VB12 appears to be due to the inability of L-perfluoroalkyl sulfonates to complex with VB12 and not an activation energy issue that can be overcome by stronger reductants/catalysts. At 90 °C, 95% of br-PFOS isomers were transformed within 5 days. Isomer-specific removal rates were positively correlated to the br-CF 3 's proximity to the terminal CF 3 . Br-PFHxS transformation was approximately two times slower with less defluorination than br-PFOS. C8/C7 and C6/C5 polyfluorinated sulfonates from br-PFOS and br-PFHxS, respectively, were identified as both intermediates and apparent dead-end products. Pathways included 4 F replaced by 2 H and a C═C bond, and serial F replacement by H with up to 12 F atoms removed from br-PFOS.

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Research works printed but not linked: 24

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Metadata

Authors
Park, S., de Perre, C., & Lee, L. S.
Affiliations
Department of Agronomy, ‡Ecological Science and Engineering, Purdue University, West Lafayette, Indiana 47907-2054, United States
ORCID
Lee, Linda S.
Venue
Environmental Science & Technology
Publisher
American Chemical Society (ACS)
Published
2017-11-20
Volume
51
Issue
23
Pages
13869-13877
ISSN
  • 0013-936X
  • 1520-5851
DOI
10.1021/acs.est.7b03744
Cited by
39
References
9
Language
en
Funders
U.S. Department of Defense (ER-2426)

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