Catalytic ozonation performance and surface property of supported Fe₃O₄ catalysts dispersions

Abstract

Fe₃O₄ was supported on mesoporous Al₂O₃ or SiO₂ (50 wt.%) using an incipient wetness impregnation method, and Fe₃O₄/Al₂O₃ exhibited higher catalytic efficiency for the degradation of 2,4-dichlorophenoxyacetic acid and para-chlorobenzoic acid aqueous solution with ozone. The effect and morphology of supported Fe₃O₄ on catalytic ozonation performance were investigated based on the characterization results of X-ray diffraction, X-ray photoelectron spectroscopy, BET analysis and Fourier transform infrared spectroscopy. The results indicated that the physical and chemical properties of the catalyst supports especially their Lewis acid sites had a significant influence on the catalytic activity. In comparison with SiO₂, more Lewis acid sites existed on the surface of Al₂O₃, resulting in higher catalytic ozonation activity. During the reaction process, no significant Fe ions release was observed. Moreover, Fe₃O₄/Al₂O₃ exhibited stable structure and activity after successive cyclic experiments. The results indicated that the catalyst is a promising ozonation catalyst with magnetic separation in drinking water treatment.

Keywords

heterogeneous catalytic ozonation / iron oxides / supports / surface Lewis acid sites

References

[1] Kasprzyk-Hordern B, Ziolek M, Nawrocki J. Catalytic ozonation and methods of enhancing molecular ozone reactions in water treatment. Applied Catalysis B: Environmental, 2003, 46(4): 639–669

[2] Benner J, Ternes T A. Ozonation of propranolol: formation of oxidation products. Environmental Science & Technology, 2009, 43(13): 5086–5093

[3] Nawrocki J, Kasprzyk-Hordern B. The efficiency and mechanisms of catalytic ozonation. Applied Catalysis B: Environmental, 2010, 99(1-2): 27–42

[4] Song S, Liu Z W, He Z Q, Zhang A L, Chen J M, Yang Y P, Xu X H. Impacts of morphology and crystallite phases of titanium oxide on the catalytic ozonation of phenol. Environmental Science & Technology, 2010, 44(10): 3913–3918

[5] Sui M H, Sheng L, Lu K X, Tian F. FeOOH catalytic ozonation of oxalic acid and the effect of phosphate binding on its catalytic activity. Applied Catalysis B: Environmental, 2010, 96(1-2): 94–100

[6] Yang L, Hu C, Nie Y L, Qu J H. Catalytic ozonation of selected pharmaceuticals over mesoporous alumina-supported manganese oxide. Environmental Science & Technology, 2009, 43(7): 2525–2529

[7] Einaga H, Futamura S. Comparative study on the catalytic activities of alumina-supported metal oxides for oxidation of benzene and cyclohexane with ozone. Reaction Kinetics and Catalysis Letters, 2004, 81(1): 121–128

[8] Liu H N, Qing B J, Ye X S, Li Q, Lee K, Wu Z J. Boron adsorption by composite magnetic particles. Chemical Engineering Journal, 2009, 151(1-3): 235–240

[9] Chen H W, Kuo Y L, Chiou C S, You S W, Ma C M, Chang C T. Mineralization of reactive Black 5 in aqueous solution by ozone/H₂O₂ in the presence of a magnetic catalyst. Journal of Hazardous Materials, 2010, 174(1-3): 795–800

[10] Lv A H, Hu C, Nie Y L, Qu J H. Catalytic ozonation of toxic pollutants over magnetic cobalt and manganese co-doped γ-Fe₂O₃. Applied Catalysis B: Environmental, 2010, 100(1-2): 62–67

[11] Lv A H, Hu C, Nie Y L, Qu J H. Catalytic ozonation of toxic pollutants over magnetic cobalt-doped Fe₃O₄ suspensions. Applied Catalysis B: Environmental, 2011, 117-118: 246–252

[12] Reddy B M, Rao K N, Bharali P. Copper promoted cobalt and nickel catalysts supported on ceria-alumina mixed oxide: Structural characterization and CO oxidation activity. Industrial & Engineering Chemistry Research, 2009, 48(18): 8478–8486

[13] Liu L J, Chen Y, Dong L H, Zhu J, Wan H Q, Liu B, Zhao B, Zhu H Y, Sun K Q, Dong L, Chen Y. Investigation of the NO removal by CO on CuO-CoO_x binary metal oxides supported on Ce₀.67Zr₀.33O₂. Applied Catalysis B: Environmental, 2009, 90(1-2): 105–114

[14] Yang L, Hu C, Nie Y L, Qu J H. Surface acidity and reactivity of β-FeOOH/Al₂O₃ for pharmaceuticals degradation with ozone: In situ ATR-FTIR studies. Applied Catalysis B: Environmental, 2010, 97(3-4): 340–346

[15] Zhao D Y, Feng J L, Huo Q S, Melosh N, Fredrickson G H, Chmelka B F, Stucky G D. Triblock copolymer syntheses of mesoporous silica with periodic 50 to 300 angstrom pores. Science, 1998, 279(5350): 548–552

[16] Ueda R, Kusakari T, Tomishige K, Fujimoto K. Nature of spilt-over hydrogen on acid sites in zeolites: Observation of the behavior of adsorbed pyridine on zeolite catalysts by means of FTIR. Journal of Catalysis, 2000, 194(1): 14–22

[17] Wandelt K. Photoemission studies of adsorbed oxygen and oxide layers. Surface Science Reports, 1982, 2(1): 1–121

[18] Temesghen W, Sherwood P. Analytical utility of valence band X-ray photoelectron spectroscopy of iron and its oxides, with spectral interpretation by cluster and band structure calculations. Analytical and Bioanalytical Chemistry, 2002, 373(7): 601–608

[19] Bulanin K M, Lavalley J C, Tsyganenko A A. IR spectra of adsorbed ozone. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 1995, 101(2-3): 153–158

[20] Al-Abadleh H A, Grassian V H. FT-IR study of water adsorption on aluminum oxide surfaces. Langmuir, 2003, 19(2): 341–347

[21] Jung H, Choi H. Catalytic decomposition of ozone and para-chlorobenzoic acid (pCBA) in the presence of nanosized ZnO. Applied Catalysis B: Environmental, 2006, 66(3-4): 288–294

RIGHTS & PERMISSIONS

Higher Education Press and Springer-Verlag Berlin Heidelberg