Abstract:a b s t r a c tFe-Al layered double hydroxides (Fe-Al LDH, the molar ratio of Fe(II) to Fe(III) was about 1:10) was successfully supported and highly dispersed on mesoporous Al 2 O 3 based on the X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) analysis. Fe-Al LDH/Al 2 O 3 was more efficient in inhibiting BrO 3 À formation and removing organic pollutant taking ozonation alone as control. Further investigation indicated that BrO 3 À reduction by surface Fe(II) was responsible to the complete i… Show more
“…The binding energy of Fe 2p 1/2 is around 724.84 eV associated with other satellite peak at 732.01 eV [68]. The peaks at around 711.01 eV and 724.84 eV, indicating Fe components were mainly in trivalent status in Fe-MCM-41 [69]. The XPS O1s peak of all the catalysts is very similar (see Figure S5).…”
Section: Characterization Of the Catalystmentioning
MCM-41 based catalysts (molar ratio Si/Al = 40) were prepared by a hydrothermal route, modified by ionic exchange with different metals (Cu, Cr, Fe and Zn) and finally calcined at 550 °C. The catalysts were fully characterized by different techniques that confirmed the formation of oxides of the different metals on the surfaces of all materials. Low-angle X-ray diffraction (XRD) analyses showed that calcination resulted in the incorporation of metallic Zn, Fe and Cr in the framework of MCM-41, while in the case of Cu, thin layers of CuO were formed on the surface of MCM-41. The solids obtained were tested in the catalytic wet peroxide oxidation (CWPO) of acetaminophen at different temperatures (25–55 °C). The activity followed the order: Cr/MCM-41 ≥ Fe/MCM-41 > Cu/MCM-41 > Zn/MCM-41. The increase of the reaction temperature improved the performance and activity of Cr/MCM-41 and Fe/MCM-41 catalysts, which achieved complete conversion of acetaminophen in short reaction times (15 min in the case of Cr/MCM-41). Fe/MCM-41 and Cr/MCM-41 were submitted to long-term experiments, being the Fe/MCM-41 catalyst the most stable with a very low metal leaching. The leaching results were better than those previously reported in the literature, confirming the high stability of Fe/MCM-41 catalysts synthesized in this study.
“…The binding energy of Fe 2p 1/2 is around 724.84 eV associated with other satellite peak at 732.01 eV [68]. The peaks at around 711.01 eV and 724.84 eV, indicating Fe components were mainly in trivalent status in Fe-MCM-41 [69]. The XPS O1s peak of all the catalysts is very similar (see Figure S5).…”
Section: Characterization Of the Catalystmentioning
MCM-41 based catalysts (molar ratio Si/Al = 40) were prepared by a hydrothermal route, modified by ionic exchange with different metals (Cu, Cr, Fe and Zn) and finally calcined at 550 °C. The catalysts were fully characterized by different techniques that confirmed the formation of oxides of the different metals on the surfaces of all materials. Low-angle X-ray diffraction (XRD) analyses showed that calcination resulted in the incorporation of metallic Zn, Fe and Cr in the framework of MCM-41, while in the case of Cu, thin layers of CuO were formed on the surface of MCM-41. The solids obtained were tested in the catalytic wet peroxide oxidation (CWPO) of acetaminophen at different temperatures (25–55 °C). The activity followed the order: Cr/MCM-41 ≥ Fe/MCM-41 > Cu/MCM-41 > Zn/MCM-41. The increase of the reaction temperature improved the performance and activity of Cr/MCM-41 and Fe/MCM-41 catalysts, which achieved complete conversion of acetaminophen in short reaction times (15 min in the case of Cr/MCM-41). Fe/MCM-41 and Cr/MCM-41 were submitted to long-term experiments, being the Fe/MCM-41 catalyst the most stable with a very low metal leaching. The leaching results were better than those previously reported in the literature, confirming the high stability of Fe/MCM-41 catalysts synthesized in this study.
“…3. From the Fe2p XPS spectra, the Fe 2p1/2 and Fe 2p3/2 peaks centered at 709.9 and 723.2 eV could be assigned to Fe (II), and the bands centered at 712.4 and 725.6 eV corresponded to the characteristic values for Fe (III) (Nie et al, 2015); in particular, a satellite peak around 718.0 eV confirmed the presence of Fe (III) species in FeC x /NCNFs. However, no signal was detected for Fe 0 at 707 eV (Nie et al, 2007).…”
Section: Characterization Of Fec X /Ncnfsmentioning
“…Recently, various advanced oxidation processes (AOPs) have been attempted to degrade 2,4-D, such as electrochemical (Zhu et al, 2012;Souza et al, 2016), electro-Fenton (Brillas et al, 2004;Casado et al, 2006), photocatalysis (Nie et al, 2015b;Mkhalid, 2016;Qiu et al, 2016), Fenton (Chen et al, 2015), ozonation (Rodríguez et al, 2017). Notably, in the late 1990s, in situ chemical oxidation (ISCO), which is based on strong oxidants such as ozone, potassium permanganate and hydrogen peroxide, has received much attention due to its effective mineralization of recalcitrant organic compounds (Devi et al, 2016;Pan et al, 2016).…”
The chlorinated phenoxy herbicide of 2,4-dichlorophenoxyacetic acid (2,4-D) was oxidized by thermally activated persulfate (TAP). This herbicide was studied for different persulfate dosages (0.97-7.29 g L), for varying initial pH levels (3-12) and temperatures (25-70 °C). Compared with Fe/PS, TAP could achieve a higher total organic carbon (TOC) removal under wider pH ranges of 3-12. Increasing the mole ratio of PS to 2,4-D favored for the decay of 2,4-D and the best performance was achieved at the ratio of 50. The 2,4-D degradation rate constant highly depended on the initial pH and temperature, in accordance with the Arrhenius model, with an apparent activation energy of 135.24 kJ mol. The study of scavenging radicals and the EPR confirmed the presence of both SO and OH. However, SO was the predominant oxidation radical for 2,4-D decay. The presence of both Cl and CO inhibited the degradation of 2,4-D, whereas the effect of NO could be negligible. Verified by GC/MS, HPLC and ion chromatography, a possible degradation mechanism was proposed.
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