New Mechanistic Aspects of the Fenton Reaction

Rachmilovich-Calis, Sandra; Masarwa, Alexandra; Meyerstein, Naomi; Meyerstein, Dan; Eldik, Rudi van

doi:10.1002/chem.200802572

Cited by 102 publications

(78 citation statements)

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“…This reaction leads to CH 4 , ethane (C 2 H 6 ), methanol and/or formaldehyde, depending on the reaction conditions [26][27][28][29] . However, under conditions used in our experiments (iron(II/III), ASC and H 2 O 2 ), when FH is replaced by water-soluble iron salts that are believed to produce hydroxyl radicals (Fenton's reaction), very little CH 4 production was observed (o1%; Supplementary Fig.…”

Section: Resultsmentioning

confidence: 99%

Abiotic methanogenesis from organosulphur compounds under ambient conditions

et al. 2014

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Methane in the environment is produced by both biotic and abiotic processes. Biomethanation involves the formation of methane by microbes that live in oxygen-free environments. Abiotic methane formation proceeds under conditions at elevated temperature and/or pressure. Here we present a chemical reaction that readily forms methane from organosulphur compounds under highly oxidative conditions at ambient atmospheric pressure and temperature. When using iron(II/III), hydrogen peroxide and ascorbic acid as reagents, S-methyl groups of organosulphur compounds are efficiently converted into methane. In a first step, methyl sulphides are oxidized to the corresponding sulphoxides. In the next step, demethylation of the sulphoxide via homolytic bond cleavage leads to methyl radical formation and finally to methane in high yields. Because sulphoxidation of methyl sulphides is ubiquitous in the environment, this novel chemical route might mimic methane formation in living aerobic organisms.

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Section: Resultsmentioning

confidence: 99%

Abiotic methanogenesis from organosulphur compounds under ambient conditions

et al. 2014

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“…The trends of the optical density and COD decreases were nearly identical, which suggested that the decoloration of MB was mainly due to the complete oxidation of MB into CO2 [20][21][22][23][24][25]. Generally, many Fenton systems generate oxidative radicals and other non-radical species [26]. To confirm the existence of ·OH radicals in the FTCNC-H 2 O 2 Fenton-like system, the electron spin resonance (ESR) spectra of the FTCNC-H 2 O 2 Fenton-like system were recorded [21].…”

Section: Decoloration Of Mb In the Ftcnc-h 2 O 2 Fenton-like Systemmentioning

confidence: 88%

“…Beyond the radical process, according to the literature, there might also be non-radical processes involved. Generally, many Fenton systems generate oxidative radicals and other non-radical species [26]. To confirm the existence of •OH radicals in the FTCNC-H2O2 Fenton-like system, the electron spin resonance (ESR) spectra of the FTCNC-H2O2 Fenton-like system were recorded [21].…”

Section: Decoloration Of Mb In the Ftcnc-h 2 O 2 Fenton-like Systemmentioning

confidence: 99%

“…Beyond the radical process, according to the literature, there might also be non-radical processes involved. Recently, van Eldik et al found a new mechanistic aspect of Fenton reactions in which not only hydroxyl radicals but also Fe III ( − O2H)aq were involved [26]. Thus, H2O2 decomposed to generate several oxidative species that further oxidized the MB molecules.…”

Section: Decoloration Of Mb In the Ftcnc-h 2 O 2 Fenton-like Systemmentioning

confidence: 99%

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Preparation of Fe3O4/TiO2/C Nanocomposites and Their Application in Fenton-Like Catalysis for Dye Decoloration

Liu

Zhang

et al. 2016

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Abstract:Fe 2+ -H 2 O 2 Fenton system is widely applied in water treatment nowadays, but the acidification and sludge generation are crucial problems to be solved. Herein, we report that Fe 3 O 4 /TiO 2 /C nanocomposites (FTCNCs) were able to catalyze the decomposition of H 2 O 2 at neutral pH and can be applied in dye decoloration. FTCNCs were prepared by precipitating TiO 2 on Fe 3 O 4 cores via the hydrolysis of tetrabutyl titanate followed by the hydrothermal dehydrogenization of glucose to deposit carbon on Fe 3 O 4 /TiO 2 . The decoloration of methylene blue (MB) in the FTCNC-H 2 O 2 Fenton-like system was monitored to reflect the catalytic activity of FTCNC. The radical generation capability was analyzed by electron spin resonance. Our results indicated that FTCNC-H 2 O 2 Fenton-like system was efficient in decolorizing MB, and the radicals led to the near complete oxidation of MB. The FTCNC-H 2 O 2 Fenton-like system could be used in a wide pH range of 4-9. A greater catalyst amount, a higher H 2 O 2 concentration, and a higher temperature accelerated the decoloration kinetics. FTCNCs showed good activity after the regeneration of 8 cycles. The implication to the practical applications of FTCNCs in water treatment is discussed.

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“…Although ubiquitous and an important source of reactive oxygen species (ROS), if HO • is indeed produced, the identity of the intermediate formed in this reaction has long been the subject of debate (Goldstein et al, 1993;MacFaul et al, 1998;Walling, 1998;Goldstein and Meyerstein, 1999;Dunford, 2002;Rachmilovich-Calis et al, 2009a;Remucal Keenan and Sedlak, 2011). It is generally accepted that HO • is formed under acidic conditions and in the absence of ligands.…”

Section: Introductionmentioning

confidence: 99%

Importance of Iron Complexation for Fenton-Mediated Hydroxyl Radical Production at Circumneutral pH

2016

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The reaction between Fe(II) and H 2 O 2 to yield hydroxyl radicals (HO • ), the Fenton reaction, is of interest due to its role in trace metal and natural organic matter biogeochemistry, its utility in water treatment and its role in oxidative cell degradation and associated human disease. There is significant dispute over whether HO • , the most reactive of the so-called reactive oxygen species (ROS), is formed in this reaction, particularly under circumneutral conditions relevant to natural systems. In this work we have studied the oxidation kinetics of Fe(II) complexed by L = citrate, ethylenediaminetetraacetic acid (EDTA) and diethylenetriaminepentaacetic acid (DTPA) and also measured HO • production using phthalhydrazide as a probe compound at pH 8.2. A kinetic model has been developed and utilized to confirm that HO • is the sole product of the Fe(II)L-H 2 O 2 reaction for L = EDTA and DTPA. Quantitative HO • production also appears likely for L = citrate, although uncertainties with the speciation of Fe(II)-citrate complexes as well as difficulties in modeling the oxidation kinetics of these complexes has prevented a definitive conclusion. In the absence of ligands at circumneutral pH, inorganic Fe(II) reacts with H 2 O 2 to yield a species other than HO • , contrary to the well-established production of HO • from inorganic Fe(II) at low pH. Our results suggest that at high pH Fe(II) must be complexed for HO • production to occur.

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New Mechanistic Aspects of the Fenton Reaction

Cited by 102 publications

References 60 publications

Abiotic methanogenesis from organosulphur compounds under ambient conditions

Abiotic methanogenesis from organosulphur compounds under ambient conditions

Preparation of Fe3O4/TiO2/C Nanocomposites and Their Application in Fenton-Like Catalysis for Dye Decoloration

Importance of Iron Complexation for Fenton-Mediated Hydroxyl Radical Production at Circumneutral pH

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