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Copper-promoted circumneutral activation of H2O2 by magnetic CuFe2O4 spinel nanoparticles: Mechanism, stoichiometric efficiency, and pathway of degrading sulfanilamide.
Chemosphere. 2016 Jul; 154:573-582.C

Abstract

To evaluate the heterogeneous degradation of sulfanilamide by external energy-free Fenton-like reactions, magnetic CuFe2O4 spinel nanoparticles (NPs) were synthesized and used as catalysts for activation of hydrogen peroxide (H2O2). The physicochemical properties of the CuFe2O4 NPs were characterized with several techniques, including X-ray diffraction, X-ray photoelectron spectroscopy, transmission electron microscopy, and magnetometry. In the catalytic experiments, CuFe2O4 NPs/H2O2 oxidation showed the best degradation performance in the circumneutral conditions that resulted from the presence of Cu(II) on the surface of the CuFe2O4 NPs. The surface area-normalized pseudo-first-order rate constants were calculated as 2.60 × 10(-2) L m(-1) min(-1), 2.58 × 10(-3) L m(-1) min(-1), 1.92 × 10(-3) L m(-1) min(-1), and 7.30 × 10(-4) L m(-1) min(-1) for CuO, CuFe2O4 NPs, Fe3O4, and α-Fe2O3 catalysts, respectively. Thus, solid state Cu(II) was more reactive and efficient than Fe(III) in the circumneutral activation of H2O2; this finding was further supported by the results regarding the stoichiometric efficiency of H2O2. The effects of experimental parameters such as the oxidant dosage and catalyst loading were investigated. The mechanism for H2O2 activation on the spinel surface was explored and could be explained by the solid redox cycles of Fe(II)/Fe(III) and Cu(II)/Cu(I). Based on the products detected, a degradation pathway via the CS bond cleavage is proposed for the degradation of sulfanilamide. The findings of this study suggest that copper can be used as a doping metal to improve the reactivity and expand the effective pH range of iron oxides.

Authors+Show Affiliations

Department of Civil Engineering, The University of Hong Kong, Pokfulam Road, Hong Kong.Department of Civil Engineering, The University of Hong Kong, Pokfulam Road, Hong Kong.Department of Civil Engineering, The University of Hong Kong, Pokfulam Road, Hong Kong. Electronic address: kshih@hku.hk.

Pub Type(s)

Journal Article

Language

eng

PubMed ID

27085318

Citation

Feng, Yong, et al. "Copper-promoted Circumneutral Activation of H2O2 By Magnetic CuFe2O4 Spinel Nanoparticles: Mechanism, Stoichiometric Efficiency, and Pathway of Degrading Sulfanilamide." Chemosphere, vol. 154, 2016, pp. 573-582.
Feng Y, Liao C, Shih K. Copper-promoted circumneutral activation of H2O2 by magnetic CuFe2O4 spinel nanoparticles: Mechanism, stoichiometric efficiency, and pathway of degrading sulfanilamide. Chemosphere. 2016;154:573-582.
Feng, Y., Liao, C., & Shih, K. (2016). Copper-promoted circumneutral activation of H2O2 by magnetic CuFe2O4 spinel nanoparticles: Mechanism, stoichiometric efficiency, and pathway of degrading sulfanilamide. Chemosphere, 154, 573-582. https://doi.org/10.1016/j.chemosphere.2016.04.019
Feng Y, Liao C, Shih K. Copper-promoted Circumneutral Activation of H2O2 By Magnetic CuFe2O4 Spinel Nanoparticles: Mechanism, Stoichiometric Efficiency, and Pathway of Degrading Sulfanilamide. Chemosphere. 2016;154:573-582. PubMed PMID: 27085318.
* Article titles in AMA citation format should be in sentence-case
TY - JOUR T1 - Copper-promoted circumneutral activation of H2O2 by magnetic CuFe2O4 spinel nanoparticles: Mechanism, stoichiometric efficiency, and pathway of degrading sulfanilamide. AU - Feng,Yong, AU - Liao,Changzhong, AU - Shih,Kaimin, Y1 - 2016/04/14/ PY - 2015/10/24/received PY - 2016/04/02/revised PY - 2016/04/06/accepted PY - 2016/4/18/entrez PY - 2016/4/18/pubmed PY - 2017/1/10/medline KW - Copper KW - CuFe(2)O(4) catalyst KW - Fenton-like KW - Mechanism KW - Sulfanilamide SP - 573 EP - 582 JF - Chemosphere JO - Chemosphere VL - 154 N2 - To evaluate the heterogeneous degradation of sulfanilamide by external energy-free Fenton-like reactions, magnetic CuFe2O4 spinel nanoparticles (NPs) were synthesized and used as catalysts for activation of hydrogen peroxide (H2O2). The physicochemical properties of the CuFe2O4 NPs were characterized with several techniques, including X-ray diffraction, X-ray photoelectron spectroscopy, transmission electron microscopy, and magnetometry. In the catalytic experiments, CuFe2O4 NPs/H2O2 oxidation showed the best degradation performance in the circumneutral conditions that resulted from the presence of Cu(II) on the surface of the CuFe2O4 NPs. The surface area-normalized pseudo-first-order rate constants were calculated as 2.60 × 10(-2) L m(-1) min(-1), 2.58 × 10(-3) L m(-1) min(-1), 1.92 × 10(-3) L m(-1) min(-1), and 7.30 × 10(-4) L m(-1) min(-1) for CuO, CuFe2O4 NPs, Fe3O4, and α-Fe2O3 catalysts, respectively. Thus, solid state Cu(II) was more reactive and efficient than Fe(III) in the circumneutral activation of H2O2; this finding was further supported by the results regarding the stoichiometric efficiency of H2O2. The effects of experimental parameters such as the oxidant dosage and catalyst loading were investigated. The mechanism for H2O2 activation on the spinel surface was explored and could be explained by the solid redox cycles of Fe(II)/Fe(III) and Cu(II)/Cu(I). Based on the products detected, a degradation pathway via the CS bond cleavage is proposed for the degradation of sulfanilamide. The findings of this study suggest that copper can be used as a doping metal to improve the reactivity and expand the effective pH range of iron oxides. SN - 1879-1298 UR - https://www.unboundmedicine.com/medline/citation/27085318/Copper_promoted_circumneutral_activation_of_H2O2_by_magnetic_CuFe2O4_spinel_nanoparticles:_Mechanism_stoichiometric_efficiency_and_pathway_of_degrading_sulfanilamide_ L2 - https://linkinghub.elsevier.com/retrieve/pii/S0045-6535(16)30493-3 DB - PRIME DP - Unbound Medicine ER -