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Tytuł:
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The Fenton Reaction in Water Assisted by Picolinic Acid: Accelerated Iron Cycling and Co-generation of a Selective Fe-Based Oxidant.
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Autorzy:
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Yang Z; State Key Laboratory of Pollution Control and Resource Reuse, School of Environment, Nanjing University, Nanjing 210023, PR China.; Department of Environmental Sciences, The Connecticut Agricultural Experiment Station, New Haven, Connecticut 06511, United States.
Shan C; State Key Laboratory of Pollution Control and Resource Reuse, School of Environment, Nanjing University, Nanjing 210023, PR China.; Research Center for Environmental Nanotechnology (ReCENT), Nanjing University, Nanjing 210023, PR China.
Pan B; State Key Laboratory of Pollution Control and Resource Reuse, School of Environment, Nanjing University, Nanjing 210023, PR China.; Research Center for Environmental Nanotechnology (ReCENT), Nanjing University, Nanjing 210023, PR China.
Pignatello JJ; Department of Environmental Sciences, The Connecticut Agricultural Experiment Station, New Haven, Connecticut 06511, United States.
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Źródło:
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Environmental science & technology [Environ Sci Technol] 2021 Jun 15; Vol. 55 (12), pp. 8299-8308. Date of Electronic Publication: 2021 May 25.
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Typ publikacji:
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Journal Article; Research Support, Non-U.S. Gov't; Research Support, U.S. Gov't, Non-P.H.S.
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Język:
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English
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Imprint Name(s):
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Publication: Washington DC : American Chemical Society
Original Publication: Easton, Pa. : American Chemical Society, c1967-
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MeSH Terms:
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Iron*
Oxidants*
Hydrogen Peroxide ; Kinetics ; Oxidation-Reduction ; Picolinic Acids ; Water
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Contributed Indexing:
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Keywords: Fenton; PICA−FeIII−OOH; autocatalysis; hydroxyl radical; iron cycling; picolinic acid
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Substance Nomenclature:
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0 (Oxidants)
0 (Picolinic Acids)
059QF0KO0R (Water)
BBX060AN9V (Hydrogen Peroxide)
E1UOL152H7 (Iron)
QZV2W997JQ (picolinic acid)
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Entry Date(s):
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Date Created: 20210525 Date Completed: 20210701 Latest Revision: 20210701
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Update Code:
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20240105
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DOI:
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10.1021/acs.est.1c00230
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PMID:
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34032409
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The Fenton reaction is limited by a narrow acidic pH range, the slow reduction of Fe(III), and susceptibility of the nonselective hydroxyl radical (HO • ) to scavenging by water constituents. Here, we employed the biodegradable chelating agent picolinic acid (PICA) to address these concerns. Compared to the classical Fenton reaction at pH 3.0, PICA greatly accelerated the degradation of atrazine, sulfamethazine, and various substituted phenols at pH 5.0 in a reaction with autocatalytic characteristics. Although HO • served as the principal oxidant, a high-spin, end-on hydroperoxo intermediate, tentatively identified as PICA-Fe III -OOH, also exhibited reactivity toward several test compounds. Chloride release from the oxidation of 2,4,6-trichlorophenol and the positive slope of the Hammett correlation for a series of halogenated phenols were consistent with PICA-Fe III -OOH reacting as a nucleophilic oxidant. Compared to HO • , PICA-Fe III -OOH is less sensitive to potential scavengers in environmental water samples. Kinetic analysis reveals that PICA facilitates Fe(III)/Fe(II) transformation by accelerating Fe(III) reduction by H 2 O 2 . Autocatalysis is ascribed to the buildup of Fe(II) from the reduction of Fe(III) by H 2 O 2 as well as PICA oxidation products. PICA assistance in the Fenton reaction may be beneficial to wastewater treatment because it favors iron cycling, extends the pH range, and balances oxidation universality with selectivity.
