紫外激活过硫酸盐降解水中双氯芬酸钠  

Degradation of diclofenac sodium in water by UV activated persulfate

作　　者：郭佑罗 高乃云[1] 关小红[1] 朱思瑞 鲁仙 安娜[1] 

机构地区：[1]污染控制与资源化研究国家重点试验室(同济大学),上海200092

出　　处：《哈尔滨工业大学学报》2017年第8期65-70,共6页Journal of Harbin Institute of Technology

基　　金：国家自然科学基金(51178321;51608372);国家科技重大专项(2012ZX07403-001;2012ZX07403-002;2008ZX07421-002);高校博士点基金(20120072110050)

摘　　要：为解决传统工艺难以有效去除水中有机污染物的问题,采用紫外激活过硫酸盐工艺去除水中典型PPCPs类物质双氯芬酸钠,考察双氯芬酸钠初始质量浓度、过硫酸盐(PS)投加量、溶液pH、阴离子质量浓度和腐殖酸(HA)投加量多种因素对紫外(UV)激活PS去除双氯芬酸钠的影响,并分析反应后中间产物可能的降解路径.结果表明:该工艺降解双氯芬酸钠与准一级动力学模型相符(R^2≥0.95),准一级反应速率常数随双氯芬酸钠初始质量浓度增加而减小,但随PS投加量的增加双氯芬酸钠的降解速率快速增大.不同的pH环境对双氯芬酸钠的降解有一定影响,溶液pH从酸性到碱性的过程中,反应速率常数的总体趋势增大.溶液中的阴离子会对系统降解双氯芬酸钠产生影响,碳酸氢根离子总体呈促进作用,氯离子呈抑制作用.HA的存在对系统去除双氯芬酸钠有较强抑制作用.SO_4^-·可能与双氯芬酸钠分子发生去羧基、去羟基等反应,主要生成N-苯基-2,6-二氯苯胺、1-(2,6-二氯苯基)-2吲哚酮、2-二氢吲哚酮及醛类物质等中间产物.To solve the deficiency of organic pollutants removal in traditional technologies, UV/persulfate （ PS ） process was employed to remove diclofenac, one of the typical pharmaceuticals and personal care products. The effect of various factors including initial diclofenac concentration, persulfate dosage, pH, inorganic anions and humic acidon the diclofenac degradation by UV/PS process was investigated. The proposed degradation pathways of intermediate products after reaction were also analyzed. The results showed that diclofenac degradation fitted the pseudo-first-order kinetics well （R^2≥0.95）. With the increase of the initial diclofenac concentration, the pseudo-first-order-constant gradually decreased. And the degradation rate of diclofenac quickly increased with the increase of the PS dosage. Different pH environment influenced the degradation rate of diclofenac to a certain extent. For the pH ranging from acidic to alkaline conditions, the degradation rate of diclofenac has an obvious increase. Inorganic anions in the solution had different degree of impact on the diclofenac degradation. The existence of bicarbonate ion accelerated the degradation but chloride ions had an adverse effect. Additionally, the existence of humic acid had an inhibition effect on the removal of diclofenac. Sulfate radicals activated by UV may react with diclofenac molecules, thereby removing carboxyl or hydroxyl herein. The main intermediate products were 2, 6-dichlorodiphenylamine, 1-（2, 6-dichlorophenyl）-2-indolinone, 2-indolinone and aldehydes or something.

关 键 词：双氯芬酸钠 动力学 过硫酸盐 速率常数 降解路径 

分 类 号：TU991[建筑科学—市政工程]