超声/过一硫酸盐氧化泛影酸钠的效果和中间产物毒性  

The oxidation performance and intermidates toxicity of sodium diatrizoate in the ultrasound activated peroxymonosulfate system

作　　者：魏红[1] 郝淼 李娟 李克斌[3] 董雯[1] 付冉 WEI Hong;HAO Miao;LI Juan;LI Kebin;DONG Wen;FU Ran(State Key Laboratory of Eco-Hydraulics in Northwest Arid Region,Xi′an University of Technology,Xi′an 710048;Shaanxi Beikong Water Co.Ltd.,Xi′an 710018;Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education,Northwest University,Xi′an 710069)

机构地区：[1]西安理工大学,西北旱区生态水利国家重点实验室,西安710048 [2]陕西北控水务有限公司,西安710018 [3]西北大学,合成与天然功能分子教育部重点实验室,西安710069

出　　处：《环境科学学报》2021年第11期4538-4546,共9页Acta Scientiae Circumstantiae

基　　金：国家自然科学基金(No.51979223);陕西省自然科学基金(No.2021JM⁃329)。

摘　　要：采用超声(Ultrasound,US)催化过硫酸氢钾(Potassium peroxymonosulfate,PMS)对离子型碘代X射线造影剂—泛影酸钠(Sodium diatrizoate,DTZ)进行氧化降解,考察反应温度、初始pH的影响,分析US/PMS氧化DTZ过程中的主要活性物质和中间产物,并采用毒理基因组学评估DTZ氧化过程中的毒性变化.结果表明,US/PMS对DTZ具有显著的氧化效果,与单独US、PMS相比,反应60 min,降解效率分别提高了18.5和1.6倍.DTZ的降解率随温度(15~45℃)的升高而升高,降解过程遵循准一级反应动力学,反应活化能E_(a)=21.98 kJ·mol^(-1);pH=3.21和9.16~11.05时,DTZ的降解率较高.自由基抑制结果和EPR分析表明,O_(2)^(-)·和^(1)O_(2)是US/PMS氧化DTZ的主要活性物质.反应过程中IO_(3)^(-)和I_(2)的生成量随DTZ降解率升高而增大.HPLC/MS/MS共检测出10种产物,其中3种为脱碘产物.基因毒理组学分析表明,DTZ毒性随反应的进行逐渐增强.Sodium diatrizoate(DTZ),one of the Ionic X⁃ray Contrast Medias,was oxidized in the ultrasound(US)-activated potassium peroxymonosulfate(PMS)system.The effect of temperature and initial pH on DTZ oxidation,the main reactive oxygen species and DTZ oxidation intermediates were identified and analyzed.In addition,the toxicity change of DTZ in the US/PMS system was assessed using the gene toxicological method.The results showed that DTZ was oxidized effectively in the US/PMS system,in 60 min,with the degradation efficiency 18.5 and 1.6 times higher than that in US and PMS individual system.DTZ degradation increased with temperature in the range of 15~45℃.The reaction followed the pseudo⁃first⁃order kinetics,and the activation energy(E_(a))was calculated as 21.98 kJ·mol^(-1).The degradation achieved higher at pH 3.21 and pH 9.16~11.05.The radical inhibition experiments and EPR results indicated that O_(2)^(-)·and^(1)O_(2)were the predominant active species responsible for DTZ oxidation.Additionally,formation of IO_(3)^(-)and I_(2)was positively related to DTZ degradation.Ten intermediate products were detected by using HPLC/MS/MS method,three of them were deiodinated products.However,the genotoxicomic results showed that DTZ toxicity was gradually enhanced with the reaction.

关 键 词：超声/过一硫酸盐 泛影酸钠 O_(2)^(-)· 1O_(2) 毒性 

分 类 号：X703[环境科学与工程—环境工程] X171.5