环境化学
姜成春,庞素艳,江进,欧阳峰,马军.无机阴离子对类-Fenton反应的影响[J].环境科学学报,2008,28(5):982-987
无机阴离子对类-Fenton反应的影响
- The effects of inorganic anions on Fenton-like reactions of atrazine and phenol
- 基金项目:国家自然科学基金资助项目(No.5047804950678104);广东省自然科学基金资助项目(No.04011215)
- 姜成春
- 深圳职业技术学院建筑与环境工程学院, 深圳 518055
- 庞素艳
- 哈尔滨工业大学深圳研究生院城市与土木工程学科部, 深圳 518055
- 江进
- 哈尔滨工业大学市政环境工程学院, 哈尔滨 150090
- 欧阳峰
- 哈尔滨工业大学深圳研究生院城市与土木工程学科部, 深圳 518055
- 马军
- 哈尔滨工业大学市政环境工程学院, 哈尔滨 150090
- 摘要:对比研究了4种常见无机阴离子(ClO4-、NO3-、Cl-和SO42-)对类-Fenton反应中H2O2分解和有机物(莠去津=2.1μmol·L-1和苯酚=50μmol·L-1)降解的影响.实验在pH=3.00±0.05(25℃)条件下完全混合反应器中进行.结果表明,在类-Fenton反应过程中,ClO4-和NO3-的存在对H2O2分解和有机物降解几乎没有影响;在不存在有机物条件下,Cl-和SO42-的加入使得H2O2分解速率显著降低,ClO4-≈NO3->Cl->SO42-;莠去津存在条件下,莠去津降解速率为ClO4-≈NO3->Cl->SO42-,而H2O2分解速率为ClO4-≈NO3-≈Cl->SO42-;苯酚存在条件下,苯酚和H2O2的降解速率为ClO4-≈NO3-≈SO42->Cl-.无机阴离子对类-Fenton反应的影响一方面是由于Cl-和SO42-与Fe3+发生络合反应,阻碍了Fe3+与H2O2络合物的形成,减少了·OH的产生;另一方面Cl-和SO42-消耗·OH,形成较低氧化活性的无机自由基(SO4·-和Cl2·-);同时,根据类-Fenton反应降解有机物的不同,无机阴离子对类-Fenton反应的影响也有所不同.
- Abstract:The effects of perchlorate,nitrate,chloride and sulfate ions on the rates of the decomposition of H2O2 and the oxidation of organic compounds([atrazine]0=2.1 μmol·L-1,[phenol]0=50 μmol·L-1) by Fenton-like processes were investigated.Experiments were conducted in a completely mixed reactor at pH=3.00±0.05(25℃).Data obtained from the Fenton-like experiments showed that the degradation rate of organics and H2O2 were not affected significantly in the presence of perchlorate and nitrate ions;whereas the presence of sulfate or chloride markedly decreased the rates of decomposition of H2O2 in the absence of organic solutes.The rates of reaction between Fe3+ and H2O2 followed the order ClO4-≈NO3->Cl->SO42-.The rates of depletion of atrazine followed the order ClO4-≈NO3->Cl->SO42- and the rates of decomposition of H2O2 in the presence of atrazine in aqueous solution were ClO4-≈NO3-≈Cl->SO42-.In the phenol system,the rates of degradation of phenol and H2O2 followed the order ClO4-≈NO3-≈SO42->Cl-.These inhibitory effects by inorganic anions are attributed to(i) the decrease of the rate of generation of hydroxyl radicals resulting from formation of complexes between Fe3+ and sulfate or chloride ions;(ii) formation of less reactive inorganic radicals(SO4·- and Cl2·-) resulting from competitive reactions between the hydroxyl radicals and sulfate or chloride ions.The impact of inorganic anions on Fenton-like reaction was also dependent on the characteristics of the model organic compounds in the system.
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