掺硼金刚石膜电极电化学氧化双酚A的影响因素及机理研究  

Influential factors and analysis of involved mechanism in electrochemical degradation of bisphenol A with boron-doped diamond electrodes

作　　者：李红娜[1] 张治国 李斌绪 叶婧[1] 张志果[2] LI Hong-na;ZHANG Zhi-guo;LI Bin-xu;YE Jing;ZHANG Zhi-guo(Institute of Environment and Sustainable Development in Agriculture,Chinese Academy of Agricultural Sciences,Beijing 100081,China;Chinese Academy of Urban Planning and Design,Beijing 100044,China)

机构地区：[1]中国农业科学院农业环境与可持续发展研究所,北京100081 [2]中国城市规划设计研究院,北京100044

出　　处：《安全与环境学报》2019年第1期254-261,共8页Journal of Safety and Environment

基　　金：国家自然科学基金项目(51308537)

摘　　要：采用响应曲面法系统研究了掺硼金刚石(Boron-doped Diamond,BDD)膜电极电化学氧化双酚A (BisphenolA,BPA)的影响因素及含氯副产物的生成。结果表明,电流密度是影响降解速率常数(k)和氯离子消耗量(Δc(Cl-))的最主要因素。以BPA有效降解的同时生成较少量的含氯副产物为标准,通过响应曲面法计算得到的最优反应条件为:对0. 06 mmol/L BPA、40 mmol/L NaCl(pH=8)的溶液,当电流密度为15 mA/cm2时,k为0. 318 min-1,Δc(Cl-)仅为3. 55 mmol/L。BDD电极电解不仅生成了高浓度的高氯酸盐,还生成了1,1,2,2-四氯乙烷、2,3,4,6-四氯苯酚和五氯苯酚等仅在BDD体系中被检测到的含氯有机副产物。综上,经BDD电极电化学氧化处理后尽管整个BPA溶液的毒性明显降低,但还需特别关注反应过程中生成的含氯副产物。The present paper is engaged in a systematic investigation and determination of the influential factors and reasons for the presence of the chlorinated byproducts in the electrochemical oxidation process of bisphenol A(BPA)with the boron-doped diamond(BDD)by using the response surface methodology(RSM)for the first time.For the said purpose,we have chosen the initial BPA concentration,the chloride concentration,the chosen pH value,and the current density as the independent variables with the degradation rate of BPA(k)and the amount of Cl-consumed(Δc(Cl-))for the targeted response.The results of our experiment prove that the current density serves as the most influential factor both on the k andΔc(Cl-),through which strong interactions have been taking place among the influential factors on these responses.It is attributed to their effects on the active chlorine,the hydroxyl radicals and the status of BPA in the electrolysis system.Based on the criteria of the effective degradation of estrogenic BPA with the relatively less generation of chlorinated byproducts,it has made us optimize the final solution with 0.06 mmol/L BPA and 40 mmol/L NaCl(pH=8)and the current density of 15 mA/cm^2 through RSM so as to get the BPA degradation rate of 0.318 min^-1 andΔc(Cl^-)of 3.55 mmol/L.The above results demonstrate the great advantages with BDD anodes compared with Pt anodes under the optimized conditions.The analysis of the specific orientation of the different forms of chlorine has been also analyzed under the different operation conditions.The active chlorine,chloroform,and perchlorate indicate the similar variation trends with the operating factors.It is indicated that the amount of chlorine consumed during the 240 min electrolysis is equal to 5.03 mmol/L for BDD anode(but only 0.30 mmol/L for Pt under the similar conditions).As a result,it emphasized that more varieties and amounts of the chlorinated byproducts in the BDD system have generated compared to the Pt system due to its stronger oxidizing capability.Besides,m

关 键 词：环境工程学 掺硼金刚石膜电极 双酚A 含氯副产物 

分 类 号：X703[环境科学与工程—环境工程]