Mechanism of PCE oxidation by percarbonate in a chelated Fe(II)-based catalyzed system

Miao, Zhouwei; Gu, Xiaoli; Lu, Shuguang; Dionysiou, Dionysios D.; Al-Abed, Souhail R.; Zang, Xueke; Wu, Xiaoliang; Qiu, Zhaofu; Sui, Qian; Danish, Muhammad

doi:10.1016/j.cej.2015.04.014

Cited by 78 publications

(26 citation statements)

References 48 publications

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“…The EPR spectrum, which has a specific quartet spectrum with peak height ratios of 1:2:2:1, indicated the formation of HO • . The results are consistent with other research [40]. The EPR detection, together with the results of the scavenging tests (Fig.…”

Section: Resultssupporting

confidence: 93%

The destruction of benzene by calcium peroxide activated with Fe(II) in water

Xue

et al. 2016

Chemical Engineering Journal

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The ability of Fe(II)-activated calcium peroxide (CaO2) to remove benzene is examined with a series of batch experiments. The results showed that benzene concentrations were reduced by 20 to 100% within 30 min. The magnitude of removal was dependent on the CaO2/Fe(II)/Benzene molar ratio, with much greater destruction observed for ratios of 4/4/1 or greater. An empirical equation was developed to quantify the destruction rate dependence on reagent composition. The presence of oxidative hydroxyl radicals (HO•) and reductive radicals (primarily O2•−) was identified by probe compound testing and electron paramagnetic resonance (EPR) tests. The results of the EPR tests indicated that the application of CaO2/Fe(II) enabled the radical intensity to remain steady for a relatively long time. The effect of initial solution pH was also investigated, and CaO2/Fe(II) enabled benzene removal over a wide pH range of 3.0~9.0. The results of radical scavenging tests showed that benzene removal occurred primarily by HO• oxidation in the CaO2/Fe(II) system, although reductive radicals also contributed. The intermediates in benzene destruction were identified to be phenol and biphenyl. The results indicate that Fe(II)-activated CaO2 is a feasible approach for treatment of benzene in contaminated groundwater remediation.

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Section: Resultssupporting

confidence: 93%

The destruction of benzene by calcium peroxide activated with Fe(II) in water

Xue

et al. 2016

Chemical Engineering Journal

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“…(5)–(6). A number of side reactions could also occur in the system that reduces the degradation efficiency [53]. Fe (II) reacts with OH% and produces Fe (III) and OH− with a rate constant of 3.0× 108 M−1s−1 (Eq.…”

Section: Resultsmentioning

confidence: 99%

Efficient transformation in characteristics of cations supported-reduced graphene oxide nanocomposites for the destruction of trichloroethane

Farooq

Danish

Brusseau

et al. 2017

Applied Catalysis A: General

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Experiments were conducted to investigate the use of graphene-oxide supported metallic nanocomposites for improving the degradation of trichloroethane (TCA) by sodium percarbonate (SPC). Two methods of production, chemical reduction (CR) and solvo-thermal (ST), were tested for preparation of single (Fe) and binary (Fe-Cu) nanocomposites supported by reduced graphene oxide (rGO). A variety of analytical techniques including N2 adsorption Brunauer-Emmett-Teller (BET), x-ray diffraction (XRD), fourier-transfrom infrared spectroscopy (FTIR), and transmisison electron microscopy (TEM) were applied to characterize the physicochemical and microstructural properties of the synthesized nanocomposites. The characterization indicated that the CR method produced nanocomposites that comprised only mesoporous structure. Conversely, both micro and mesoporous structures were present for samples produced with the ST method. The synthesized single and bimetallic composites produced from the ST method showed higher surface areas, i.e. 93.6 m2/g and 119.2 m2/g as compared to the ones synthesized via the CR method, i.e. 13.8 m2/g and 38.0 m2/g respectively. The results of FTIR and XRD analyses confirmed that the ST method produced highly crystalline nanocomposites. SEM and TEM analysis validated that metallic particles with definite morphology well distributed on the surface of rGO. X-ray photoelectron spectroscopy (XPS) analysis confirmed the homogeneity nanocomposites and occurrence of variation in copper oxidation states during degradation process. EDS mapping validate the homogeneous distribution of Cu and Fe at reduced graphene oxide surface. The Fe-Cu/rGO (ST) activated SPC system effectively degraded TCA (92%) in 2.5 h at low nanocomposite dose compared to the Fe-Cu/rGO (CR) and only Fe, for which the maximum degradation efficiencies achieved were 81% and 34%. In conclusion, excellent catalytic characteristics were observed for the ST-synthesized single and bimetallic (Fe/rGO, Fe-Cu/rGO) catalysts. These catalysts were successful in improving the degradation of TCA via activated SPC.

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“…O 2 •− is a weak reductant that reacts with CT at a rate constant of 3800 M −1 s −1 in dimethyl sulfoxide and it is documented that O 2 •− can reduce CT in Fenton-like systems [36]. Our previous study has demostrated the presence of O 2 •− in CIT and OA modified Fe(II)/SPC systems [37]. Therefore, it is quite possible that the oxidation and reduction reactions contributing to the degradation of contaminants may simultaneously occur in the Fe(III)/SPC or CAs modified Fe(III)/SPC systems.…”

Section: Resultsmentioning

confidence: 99%

Enhancement effects of chelating agents on the degradation of tetrachloroethene in Fe(III) catalyzed percarbonate system

Miao¹,

et al. 2015

Chemical Engineering Journal

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The performance of Fe(III)-based catalyzed sodium percarbonate (SPC) for stimulating the oxidation of tetrachloroethene (PCE) for groundwater remediation applications was investigated. The chelating agents citric acid monohydrate (CIT), oxalic acid (OA), and Glutamic acid (Glu) significantly enhanced the degradation of PCE. Conversely, ethylenediaminetetraacetic acid (EDTA) had a negative impact on PCE degradation, which may due to its strong Fe chelation and HO• scavenging abilities. However, excessive SPC or chelating agent will retard PCE degradation. In addition, investigations using free radical probe compounds and radical scavengers revealed that PCE was primarily degraded by HO• radical oxidation in both the chelated and non-chelated systems, while O2•− also participated in the non-chelated system and the OA and Glu modified systems. According to the electron paramagnetic resonance (EPR) studies, the presence of HO• in the Fe(III)/SPC system was maintained much longer than that in the Fe(II)/SPC system. The results indicated that the addition of CIT, OA or Glu indeed enhanced the generation of HO• in the first 10 min and promoted degradation efficiency by increasing the amount of Fe(III) and maintaining the concentration of HO• radicals in solution. In conclusion, chelated Fe(III)-based catalyzed SPC oxidation is a promising method for the remediation of PCE-contaminated groundwater.

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Mechanism of PCE oxidation by percarbonate in a chelated Fe(II)-based catalyzed system

Cited by 78 publications

References 48 publications

The destruction of benzene by calcium peroxide activated with Fe(II) in water

The destruction of benzene by calcium peroxide activated with Fe(II) in water

Efficient transformation in characteristics of cations supported-reduced graphene oxide nanocomposites for the destruction of trichloroethane

Enhancement effects of chelating agents on the degradation of tetrachloroethene in Fe(III) catalyzed percarbonate system

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