Mineralization of pentachlorophenol by ferrioxalate-assisted solar photo-Fenton process at mild pH

Ye, Zhihong; Sirés, Ignasi; Zhang, Hui; Huang, Yao Hui

doi:10.1016/j.chemosphere.2018.10.221

Cited by 39 publications

(3 citation statements)

References 37 publications

(41 reference statements)

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“…Note that, in this kind of complex water matrix, the oxidation of Cl − anion at the anode surface yields additional oxidants like active chlorine (Cl2 and ClO − ) along with chlorine radicals (Table S1) (Panizza and Cerisola, 2009). Carboxylates like oxalate and citrate have been two widely used chelating agents in non-electrochemical Fenton treatments (Ye et al, 2019c). However, polydentate ligands like nitrilotriacetic (NTA), ethylenediaminetetraacetic (EDTA) and ethylenediamine-N,N'-disuccinic (EDDS) acids seem more interesting to ensure iron complexation (Clarizia et al 2017).…”

Section: Introductionmentioning

confidence: 99%

Expanding the application of photoelectro-Fenton treatment to urban wastewater using the Fe(III)-EDDS complex

Brillas

Centellas

et al. 2020

Water Research

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This work reports the first investigation on the use of EDDS as chelating agent in photoelectro-Fenton (PEF) treatment of water at near-neutral pH. As a case study, the removal of the antidepressant fluoxetine was optimized, using an electrochemical cell composed of an IrO2-based anode an air-diffusion cathode for in-situ H2O2 production. Electrolytic trials at constant current were made in ultrapure water with different electrolytes, as well as in urban wastewater (secondary effluent) at pH 7.2. PEF with Fe(III)-EDDS (1:1) complex as catalyst outperformed electro-Fenton and PEF processes with uncomplexed Fe(II) or Fe(III). This can be explained by: (i) the larger solubilization of iron ions during the trials, favoring the production of • OH from Fenton-like reactions between H2O2 and Fe(II)-EDDS or Fe(III)-EDDS, and (ii) the occurrence of Fe(II) regeneration from Fe(III)-EDDS photoreduction, which was more efficient than conventional photo-Fenton reaction with uncomplexed Fe(III). The greatest drug concentration decays were achieved at low pH, using only 0.10 mM Fe(III)-EDDS in a 1:1 molar ratio, although complete removal in wastewater was feasible only with 0.20 mM Fe(III)-EDDS due to the greater formation of • OH. The effect of the applied current and anode nature was rather insignificant. A progressive destruction of the catalytic complex was unveiled, whereupon the mineralization mainly progressed thanks to the action of • OH adsorbed on the anode surface. Despite the incomplete mineralization using BDD as the anode, a remarkable toxicity decrease was determined. Fluoxetine degradation yielded F − and NO3 − ions, along with several aromatic intermediates. These included two chloroorganics, as a result of the anodic oxidation of Cl − to active chlorine. A detailed mechanism for the Fe(III)-EDDS-catalyzed PEF treatment of fluoxetine in urban wastewater is finally proposed.

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Section: Introductionmentioning

confidence: 99%

Expanding the application of photoelectro-Fenton treatment to urban wastewater using the Fe(III)-EDDS complex

Brillas

Centellas

et al. 2020

Water Research

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“…Accordingly, unconventional approaches have been developed, including heterogeneous Fenton treatments with solid iron catalysts (Ye et al 2020b) and homogeneous processes with soluble chelated iron (Clarizia et al 2017;Ganiyu et al 2018). In previous work, some of us explored the viability of chelators like oxalate for pentachlorophenol degradation by solar photo-Fenton (Ye et al 2019c) and ethylenediamine-N,N'-disuccinic acid (EDDS) to destroy butylated hydroxyanisole by EF (Ye et al 2019a) and fluoxetine by PEF (Ye et al 2020a). EDDS has been found more interesting because of its biodegradability and the high efficiency of Fe(III)-EDDS-catalyzed treatments at neutral pH (Miralles-Cuevas et al 2019).…”

Section: Introductionmentioning

confidence: 99%

Photoelectro-Fenton treatment of pesticide triclopyr at neutral pH using Fe(III)–EDDS under UVA light or sunlight

Soares

Oriol

et al. 2020

Environ Sci Pollut Res

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One of the main challenges of electrochemical Fenton-based processes is the treatment of organic pollutants at near-neutral pH. As a potential approach to this problem, this work addresses the use of a low content of soluble chelated metal catalyst, formed between Fe(III) and ethylenediamine-N,N'-disuccinic (EDDS) acid (1:1), to degrade the herbicide triclopyr in 0.050 M Na2SO4 solutions at pH 7.0 by photoelectro-Fenton with UVA light or sunlight (PEF and SPEF, respectively). Comparison with electro-Fenton treatments revealed the crucial role of the photo-Fenton-like reaction, since this promoted the production of soluble Fe(II) that enhanced the pesticide removal. Hydroxyl radicals formed at the anode surface and in the bulk were the main oxidants. A boron-doped diamond (BDD) anode yielded a greater mineralization than an IrO2-based one, at the expense of reduced cost-effectiveness. The effect of catalyst concentration and current density on the performance of PEF with BDD was examined. The PEF trials in 0.25 mM Na2SO4 + 0.35 mM NaCl medium showed a large influence of generated active chlorine as oxidant, being IrO2 more suitable than RuO2 and BDD.In SPEF with BDD, the higher light intensity from solar photons accelerated the removal of the catalyst and triclopyr, with small effect on mineralization. A plausible route for the herbicide degradation by Fe(III)-EDDS-catalyzed PEF and SPEF is finally proposed based on detected byproducts: three heteroaromatic and four linear N-aliphatic compounds, formamide and tartronic and oxamic acids.

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“…The photoferrioxalate system (PFS) [Fe(III)(C 2 O 4 )] 3– has been used innumerable times for the chemical actinometry in liquid systems. − Recently, it has been extensively applied in wastewater and environment treatment. − The photolysis of PFS generates various reactive intermediates, such as Fe(II) and reactive oxygen species (ROS), including O •– , • OH, and H 2 O 2 , that are significant for the oxidative decontamination of organic substances in the environment and engineered systems. This photoreduction is conventionally expressed as 2 false[ Fe ( III ) false( normalC 2 normalO 4 false) 3 false] 3 − + h ν → 2 false[ Fe ( II ) false( normalC 2 normalO 4 false) 2 false] 2 − + 2 CO 2 + ( C 2 O 4 ) 2 − Understanding its prime mechanisms is crucial to optimizing the reactive paths and to controlling their outcomes.…”

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Exploring Ligand-to-Metal Charge-Transfer States in the Photo-Ferrioxalate System Using Excited-State Specific Optimization

Tran,

Neuscamman

2023

J. Phys. Chem. Lett.

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The photo-ferrioxalate system (PFS), [Fe(III)(C 2 O 4 )] 3− , more than an exact chemical actinometer, has been extensively applied in wastewater and environment treatment. Despite many experimental efforts to improve clarity, important aspects of the mechanism of ferrioxalate photolysis are still under debate. In this paper, we employ the recently developed WΓ-CASSCF to investigate the ligand-to-metal charge-transfer states that are key to ferrioxalate photolysis. This investigation provides a qualitative picture of these states and key potential energy surface features related to the photolysis. Our theoretical results are consistent with the prompt charge-transfer picture seen in recent experiments and clarify some features that are not visible in experiments. Two ligand-to-metal charge-transfer states contribute to the photolysis of ferrioxalate, and the avoided crossing barrier between them is low compared with the initial photoexcitation energy. Our data also clarify that one Fe−O bond cleaves first, followed by the C−C bond and the other Fe−O bond.

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Mineralization of pentachlorophenol by ferrioxalate-assisted solar photo-Fenton process at mild pH

Cited by 39 publications

References 37 publications

Expanding the application of photoelectro-Fenton treatment to urban wastewater using the Fe(III)-EDDS complex

Expanding the application of photoelectro-Fenton treatment to urban wastewater using the Fe(III)-EDDS complex

Photoelectro-Fenton treatment of pesticide triclopyr at neutral pH using Fe(III)–EDDS under UVA light or sunlight

Exploring Ligand-to-Metal Charge-Transfer States in the Photo-Ferrioxalate System Using Excited-State Specific Optimization

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