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微波辐射强化UV/H2O2体系中苯酚的氧化分解及动力学研究

Improvement of oxidative decomposition of aqueous phenol by microwave irradiation in UV/H2O2 process and kinetic study.

作者信息

Han Do-Hung, Cha Sang-Yeob, Yang Hae-Young

机构信息

School of Chemical Engineering and Technology, Yeungnam University, 214-1 Gyongsan, Gyongbuk 712-749, South Korea.

出版信息

Water Res. 2004 Jun;38(11):2782-90. doi: 10.1016/j.watres.2004.03.025.

Abstract

2.5GHz of microwave irradiation can cause a considerable improvement of oxidative decomposition of aqueous phenol in a UV/H2O2 system. The experimental results showed that the microwave irradiation can raise both the phenol conversion and the TOC removal efficiency up to or above 50%. Also, the microwave irradiation could considerably enhance the oxidative degradation of phenol in the UV/H2O2 system even under a suppression of thermal effect. Addition of hydrogen peroxide by more than a stoichiometric amount was critical to mineralize aqueous phenol to create a short reaction time. Also, microwave irradiation can accelerate the degradation rate of intermediates, hydroquinone and catechol, produced in the course of phenol oxidative decomposition. From the kinetic study, the disappearance rate of phenol can be expressed as dX/dt = kPH[M]0(alpha - X)(1 - X), where alpha equivalent [H2O2]0/[M]0 + kOH[OH*]/kPH[M]0, shows a good correlation with the experimental data. The kinetic analysis showed that an indirect reaction of phenol with OH radical might be dominant in the absence of microwave irradiation, meanwhile a direct reaction of phenol with hydrogen peroxide might be dominant in the presence of microwave irradiation except for low concentrations of hydrogen peroxide.

摘要

2.5吉赫兹的微波辐射可使紫外/过氧化氢体系中苯酚水溶液的氧化分解有显著改善。实验结果表明,微波辐射可使苯酚转化率和总有机碳去除效率提高到50%或以上。此外,即使在热效应受到抑制的情况下,微波辐射也能显著增强紫外/过氧化氢体系中苯酚的氧化降解。加入超过化学计量比的过氧化氢对于使苯酚水溶液矿化以缩短反应时间至关重要。此外,微波辐射可加速苯酚氧化分解过程中产生的中间体对苯二酚和邻苯二酚的降解速率。从动力学研究来看,苯酚的消失速率可表示为dX/dt = kPH[M]0(α - X)(1 - X),其中α等于[H2O2]0/[M]0 + kOH[OH*]/kPH[M]0,与实验数据具有良好的相关性。动力学分析表明,在无微波辐射时,苯酚与羟基自由基的间接反应可能占主导,而在有微波辐射时,除了过氧化氢浓度较低的情况外,苯酚与过氧化氢的直接反应可能占主导。

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