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The DOI matches its Crossref record; 10 of the 10 references it cites were found in a registry or an index.

Reductive defluorination of branched per-and polyfluoroalkyl substances with cobalt complex catalysts

Liu, Jinyong, Van Hoomissen, Daniel J., Liu, Tianchi, Maizel, Andrew, Huo, Xiangchen, Fernández, Seth R., Ren, Changxu, Xiao, Xin, Fang, Yida, Schaefer, Charles E., Higgins, Christopher P., Vyas, Shubham, Strathmann, Timothy J.·2018·Environmental Science & Technology Letters
DOI 10.1021/acs.estlett.8b00122
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Abstract

This study investigates structure–reactivity relationships within branched per- and polyfluoroalkyl substances (PFASs) undergoing cobalt-catalyzed reductive defluorination reactions. Experimental results and theoretical calculations reveal correlations among the extent of PFAS defluorination, the local C–F bonding environment, and calculated bond dissociation energies (BDEs). In general, BDEs increase in the following order: tertiary C–F bonds < secondary C–F bonds < primary C–F bonds. A tertiary C–F bond adjacent to three fluorinated carbons (or two fluorinated carbons and one carboxyl group) has a relatively low BDE that permits an initial defluorination to occur. Both a biogenic cobalt–corrin complex (B 12 ) and an artificial cobalt–porphyrin complex (Co- PP ) are found to catalytically defluorinate multiple C–F bonds in selected PFASs. In general, Co- PP exhibits an initial rate of defluorination that is higher than that of B 12 . Neither complex induced significant defluorination in linear perfluorooctanoic acid (PFOA; no tertiary C–F bond) or a perfluoroalkyl ether carboxylic acid (tertiary C–F BDEs too high). These results open new lines of research, including (1) designing branched PFASs and cobalt complexes that promote complete defluorination of PFASs in natural and engineered systems and (2) evaluating potential impacts of branched PFASs in biological systems where B 12 is present.

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Metadata

Authors
Liu, J., Van Hoomissen, D. J., Liu, T., Maizel, A., Huo, X., Fernández, S. R., Ren, C., Xiao, X., Fang, Y., Schaefer, C. E., Higgins, C. P., Vyas, S., & Strathmann, T. J.
Affiliations
  • Department of Chemical and Environmental Engineering, University of California, Riverside, California 92521, United States
  • Department of Environmental Science, Zhejiang University, Hangzhou 310058, China
  • CDM Smith, 110 Fieldcrest Avenue, No. 8, Sixth Floor, Edison, New Jersey 08837, United States
ORCID
Venue
Environmental Science & Technology Letters
Publisher
American Chemical Society (ACS)
Published
2018-03-28
Volume
5
Issue
5
Pages
289-294
ISSN
2328-8930
DOI
10.1021/acs.estlett.8b00122
Cited by
98
References
10
Language
en
Funders
  • Division of Chemistry (CHE-1709719, CHE-1710079)
  • U.S. Environmental Protection Agency (ER-2424)
  • U.S. Department of Defense (ER-2424)
  • China Scholarship Council
  • U.S. Department of Energy (ER-2424)

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