Ye Miaomiao, Chen Zhonglin, Liu Xiaowei, Ben Yue, Shen Jimin
State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology, Harbin, PR China.
J Hazard Mater. 2009 Aug 15;167(1-3):1021-7. doi: 10.1016/j.jhazmat.2009.01.091. Epub 2009 Jan 31.
The TiO(2)/UV/O(3) process has been employed to remove 4-chloronitrobenzene (4-CNB) and compared to UV/air, O(3), TiO(2)/O(3), TiO(2)/UV/O(2) and UV/O(3) five parallel oxidation pathways. The reaction activities of these six processes were tested in aqueous using electron paramagnetic resonance (EPR) spin trapping technique with 5,5-dimethyl-1-pyrroline N-oxide (DMPO) spin trap. Moreover, the effects of ozone dosage, catalyst dosage and initial solution pH on the degradation of 4-CNB by TiO(2)/UV/O(3) process were also investigated. Results showed that the TiO(2)/UV/O(3) is the most efficient process for complete mineralization of 4-CNB since the combination of photocatalytic oxidation with ozone has a synergistic effect. The relative intensity of DMPO-OH follows the order of UV/air<O(3)<TiO(2)/O(3)<UV/O(3)<TiO(2)/UV/O(2)<TiO(2)/UV/O(3). In TiO(2)/UV/O(3) process, the ozone and catalyst dosage are found to have a significant impact on the process efficiency whereas initial pH has relatively less effect. Chlorine atoms of 4-CNB are absolutely oxidized to chloride anions when the ozone dosage in the range of 5-18 mg/min, or the catalyst dosage ranging from 1.0 to 2.0 g/L. Part of chloride anions would be further oxidized to chlorate(V) ions if the ozone dosage exceeds 24 mg/min, or the catalyst dosage exceeds 2.0 g/L.
TiO(2)/UV/O(3)工艺已被用于去除4-氯硝基苯(4-CNB),并与UV/空气、O(3)、TiO(2)/O(3)、TiO(2)/UV/O(2)和UV/O(3)这五条平行氧化途径进行了比较。使用5,5-二甲基-1-吡咯啉N-氧化物(DMPO)自旋捕集剂,通过电子顺磁共振(EPR)自旋捕集技术在水溶液中测试了这六种工艺的反应活性。此外,还研究了臭氧剂量、催化剂剂量和初始溶液pH值对TiO(2)/UV/O(3)工艺降解4-CNB的影响。结果表明,TiO(2)/UV/O(3)是实现4-CNB完全矿化的最有效工艺,因为光催化氧化与臭氧的结合具有协同效应。DMPO-OH的相对强度顺序为UV/空气<O(3)<TiO(2)/O(3)<UV/O(3)<TiO(2)/UV/O(2)<TiO(2)/UV/O(3)。在TiO(2)/UV/O(3)工艺中,发现臭氧和催化剂剂量对工艺效率有显著影响,而初始pH值的影响相对较小。当臭氧剂量在5-18mg/min范围内或催化剂剂量在1.0-2.0g/L范围内时,4-CNB中的氯原子完全被氧化为氯离子。如果臭氧剂量超过24mg/min或催化剂剂量超过2.0g/L,部分氯离子会进一步被氧化为氯酸根(V)离子。