Effect of TiO2 crystal phase on oxidation efficiency of H2O2/O3

被引：0

作者：

Ni, Jinlei ^{[1
]}

Peng, Ruofan ^{[1
]}

Tong, Shaoping ^{[1
]}

Ma, Chun'an ^{[1
]}

机构：

[1] State Key Laboratory Breeding Base of Green Chemistry-Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310032, Zhejiang

来源：

Huagong Xuebao/CIESC Journal | 2015年 / 66卷 / 10期

基金：

中国国家自然科学基金;

关键词：

Catalyst; Crystal phase; Hydrogen peroxide; Oxidation; Ozone; Radical; Titanium dioxide;

D O I：

10.11949/j.issn.0438-1157.20141858

中图分类号：

学科分类号：

摘要：

The oxidation efficiency of H2O2/O3 catalyzed by titanium dioxide (TiO2) for acetic acid (HAc) degradation, a probe compound for hydroxyl radical in ozonation, was investigated, with a focus on the effect of TiO2 crystal phase. The results indicated that the addition of TiO2 showed negative effect on the oxidation efficiency when the initial pH was at 7.0 and 10.0, and among all crystal phases of TiO2 anatase had the biggest negative effect. However, when the initial pH was at 3.0, rutile could significantly improve the oxidation efficiency of the H2O2/O3 system, and anatase had negligible effect. The mechanism study showed that there existed a good correlation between degradation rate of HAc and concentration of H2O2 (or its decomposition rate). Both anatase and rutile could accelerate decomposition of H2O2 at initial pH of 7.0 and 10.0, and faster was for the former than the latter. Too high decomposition rate of H2O2 could reduce removal rate of HAc at the two pH, because the conjugate base HO2- of H2O2 generated could react with ozone to effectively produce hydroxyl radicals (•OH). At initial pH 3.0, the oxidation efficiency of H2O2/O3 system was very low due to the difficulty of H2O2 deprotonation, so the concentration of H2O2 had almost no change. Addition of TiO2 could markedly accelerate the decomposition rate of H2O2, including deprotonation step, and anatase made H2O2 decomposition finish in 5 min and too fast, leading to have no effect on the oxidation efficiency. However, rutile had no such high decomposition rate for H2O2 and could generate HO2--similar species which could react with ozone to produce hydroxyl radicals (•OH) to degrade acetic acid. The batch test carried out also gave a similar result. Therefore, it can be concluded that suitable initiator and its concentration may play an important role in ozone-based advanced oxidation process, and that too high concentration of initiator might lead to rapid consumption of oxidants. The amounts of superoxide ion radical (•O2-) in H2O2/O3, anatase TiO2/H2O2/O3 and rutile TiO2/H2O2/O3 systems were determined by capturing method of Nitro Blue Tetrazolium Chloride (NBT), the order was as follows: H2O2/O3<rutile TiO2/H2O2/O3<anatase TiO2/H2O2/O3, which was in accord with the results of the results of HAc degradation. © All right reserved.

引用

页码：3950 / 3956

页数：6

共 30 条

[1]

Legube B., Leitner N.K.V., Catalytic ozonation: A promising advanced oxidation technology for water treatment, Catalysis Today, 53, 1, pp. 61-72, (1999)

[2]

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

[3]

Zeng Z.Q., Wang J.F., Li Z.H., Sun B.C., Shao L., Li W.J., Chen J.F., Zou H.K., The advanced oxidation process of phenol solution by O3/H2O2 in a rotating packed bed, Ozone: Science & Engineering, 35, 2, pp. 101-108, (2013)

[4]

Nawrocki J., Catalytic ozonation in water: Controversies and questions. discussion paper, Applied Catalysis B: Environmental, 142-143, pp. 465-471, (2013)

[5]

Pines D.S., Reckhow D.A., Effect of dissolved cobalt(II) on the ozonation of oxalic acid, Environmental Science and Technology, 36, 19, pp. 4046-4051, (2002)

[6]

Beltran F.J., Rivas F.J., Montero-De-Espinosa R., Iron type catalysts for the ozonation of oxalic acid in water, Water Research, 39, 15, pp. 3553-3564, (2005)

[7]

Li W., Liu P., Zhang H., Shi R., Tong S., Ma C., Degradation of acetic acid by Ti(IV)-catalyzed H2O2/O3, CIESC Journal, 61, 7, pp. 1790-1795, (2010)

[8]

Tong S.P., Zhao S.Q., Lan X.F., Ma C.A., A kinetic model of Ti(IV)-catalyzed H2O2/O3 process in aqueous solution, Journal of Environmental Sciences, 23, 12, pp. 2087-2092, (2011)

[9]

Xiao H., Liu R.P., Zhao X., Qu J.H., Enhanced degradation of 2, 4-dinitrotoluene by ozonation in the presence of manganese(II) and oxalic acid, Journal of Molecular Catalysis A: Chemical, 286, 1-2, pp. 149-155, (2008)

[10]

Dorota B.M., Jacek S., Stanislaw L., Kinetic studies of n-butylparaben degradation in H2O2/UV system, Ozone: Science & Engineering, 34, 5, pp. 354-358, (2012)

← 1 2 3 →