TY - JOUR
T1 - Reactivity of novel Ceria–Perovskite composites CeO2- LaMO3 (MCu, Fe) in the catalytic wet peroxidative oxidation of the new emergent pollutant ‘Bisphenol F’
T2 - Characterization, kinetic and mechanism studies
AU - Hammouda, Samia Ben
AU - Zhao, Feiping
AU - Safaei, Zahra
AU - Babu, Indu
AU - Ramasamy, Deepika Lakshmi
AU - Sillanpää, Mika
N1 - Publisher Copyright:
© 2017 Elsevier B.V.
PY - 2017
Y1 - 2017
N2 - In the present study, ceria, pristine perovskites LaMO3 (Cu, Fe) and novel ceria-perovskite composites CeO2-LaMO3 were successfully prepared and applied as heterogeneous Fenton like- catalysts for the degradation and mineralization of a new emergent compound- bisphenol F (BPF) in aqueous solution. The catalysts were characterized by X-ray diffraction spectrometer (XRD), BET surface area determination, scanning electron microscopy (SEM), Energy Dispersive X-ray (EDS) and X-ray photoelectron spectroscopy (XPS) techniques. Catalytic bisphenol F behavior shows that the activity of pristine perovskites was improved due to the introduction of cerium. Catalytic activity in terms of TOC removal followed the order of CeO2-LaCuO3 > CeO2-LaFeO3 > LaCuO3 > LaFeO3 > CeO2 with about 83, 79, 68, 64 and 28% respectively. Only the novel composite oxide CeO2-LaCuO3 was found to be effective for Bisphenol F degradation at neutral conditions. EPR analyses and scavenging experiments revealed that BPF was mainly decomposed by the attack of [rad]OH, especially the surface-bounded [rad]OH. BPF decay followed pseudo-first-order reaction kinetics. The absolute rate constant for BPF oxidation by [rad]OH was found to 2.09109 M−1 s−1, as determined by the competition kinetic method. Six stable organics intermediates were observed and five of them were identified p-benzoquinone, hydroquinone, 4-hydroxybenzaldehyde and Bis (4-hyroxyphenyl) methanol. Subsequent attack of these intermediates by [rad]OH radicals led to the formation of short chain acids: malonic, succinic, acetic, formic and oxalic acids. On the basis of the analytical results for the intermediate products and the assumption that hydroxyls radicals are the major reactive species, a plausible pathway of BPF mineralization during the heterogeneous Fenton process was proposed. Furthermore, the CeO2-LaCuO3 composite exhibited excellent long-term stability in the heterogeneous Fenton-like process. These results suggested that the novel ceria perovskite material would be a promising candidate for practical wastewater treatment.
AB - In the present study, ceria, pristine perovskites LaMO3 (Cu, Fe) and novel ceria-perovskite composites CeO2-LaMO3 were successfully prepared and applied as heterogeneous Fenton like- catalysts for the degradation and mineralization of a new emergent compound- bisphenol F (BPF) in aqueous solution. The catalysts were characterized by X-ray diffraction spectrometer (XRD), BET surface area determination, scanning electron microscopy (SEM), Energy Dispersive X-ray (EDS) and X-ray photoelectron spectroscopy (XPS) techniques. Catalytic bisphenol F behavior shows that the activity of pristine perovskites was improved due to the introduction of cerium. Catalytic activity in terms of TOC removal followed the order of CeO2-LaCuO3 > CeO2-LaFeO3 > LaCuO3 > LaFeO3 > CeO2 with about 83, 79, 68, 64 and 28% respectively. Only the novel composite oxide CeO2-LaCuO3 was found to be effective for Bisphenol F degradation at neutral conditions. EPR analyses and scavenging experiments revealed that BPF was mainly decomposed by the attack of [rad]OH, especially the surface-bounded [rad]OH. BPF decay followed pseudo-first-order reaction kinetics. The absolute rate constant for BPF oxidation by [rad]OH was found to 2.09109 M−1 s−1, as determined by the competition kinetic method. Six stable organics intermediates were observed and five of them were identified p-benzoquinone, hydroquinone, 4-hydroxybenzaldehyde and Bis (4-hyroxyphenyl) methanol. Subsequent attack of these intermediates by [rad]OH radicals led to the formation of short chain acids: malonic, succinic, acetic, formic and oxalic acids. On the basis of the analytical results for the intermediate products and the assumption that hydroxyls radicals are the major reactive species, a plausible pathway of BPF mineralization during the heterogeneous Fenton process was proposed. Furthermore, the CeO2-LaCuO3 composite exhibited excellent long-term stability in the heterogeneous Fenton-like process. These results suggested that the novel ceria perovskite material would be a promising candidate for practical wastewater treatment.
KW - Bisphenol F
KW - Ceria
KW - Fenton
KW - Heterogeneous
KW - Perovskite
UR - http://www.scopus.com/inward/record.url?scp=85021155808&partnerID=8YFLogxK
U2 - 10.1016/j.apcatb.2017.06.047
DO - 10.1016/j.apcatb.2017.06.047
M3 - Article
AN - SCOPUS:85021155808
SN - 0926-3373
VL - 218
SP - 119
EP - 136
JO - Applied Catalysis B: Environmental
JF - Applied Catalysis B: Environmental
ER -