针对废弃药物绿色处理技术匮乏的实际问题,以双氯芬酸钠(DS)药物为研究对象,探讨了碱催化水热氧化法对其的无害化处理效果,确定了相应的操作方法并优化了反应参数.利用单因素实验确定了适宜的实验因素水平,通过响应面分析法进一步解析优化了多因素交互作用下的反应条件.结果表明,碱催化水热氧化法能有效通过脱氯过程实现DS的无害化处理,最佳反应参数为:H2O2:DS0.3mL/mg、反应时间98min、反应温度196℃,脱氯效率优化值为99.6%,实测值为98.9%,相对误差0.70%.通过降解产物测定和解析,发现碱催化水热氧化处理DS存在2个反应路径:(1)苯环之间C-N键断裂,然后氧化开环脱氯;(2)苯环上直接羟基化,然后氧化开环脱氯.本研究为废弃DS类药物的无害化处理提供了一条绿色环保的新途径.
Aiming at the problem of lacking of green treatment technologies for pharmaceutical wastes,the current study was carried out to investigate the detoxification effect of base-catalyzed hydrothermal oxidation on diclofenac sodium(DS)medicine.The corresponding operation method was established and the reaction parameters were optimized.The suitable experimental levels were determined by single-factor design,and response surface methodology(RSM)was carried out to further establish the optimum conditions under multi-factor interaction.The results showed that base-catalyzed hydrothermal oxidation was an efficient approach for the detoxification of DS by dechlorination.The optimal parameters were,H2O2:DS0.3mL/mg,reaction time98min,reaction temperature196℃,respectively.It was noted that the determined value was98.9%and the predicted value was99.6%with a relative error of0.70%.Determination and analysis of the degradation products showed that there were two different reaction pathways for the degradation of DS by base-catalyzed hydrothermal oxidation:(1)the C-N bond between the two benzene rings cleaved,followed by benzene rings opened and dechlorinated through oxidation;(2)the benzene rings directly hydroxylated,followed by benzene rings opened and dechlorinated through oxidation.This study provides a green and environmentally benign approach for the detoxification of waste DS medicine.