摘要
针对污水处理厂尾水中抗生素等生物难降解有机物频繁检出的问题,采用相对绿色、低毒性的过渡金属元素制备了锰铁铜类水滑石(MnFeCu-LDHs),并将其用于活化过一硫酸盐(PMS)降解氯四环素(CTC)。探究了初始pH、反应温度、催化剂和PMS投量对CTC降解效能的影响规律,通过化学捕获和淬灭实验确定了活性氧物种(ROS)的种类与贡献,并对反应前后的催化剂进行理化性质表征且考察了催化剂稳定性。结果表明,在初始pH为7、反应温度为298 K、催化剂及PMS投加量均为0.2 g·L^(-1)条件下,反应5 min后CTC去除率达到80.88%,30 min去除率达到91.18%,同时,随着初始pH和温度的提高,CTC的降解效果得到明显增强;ROS淬灭实验和EPR捕获实验结果证实了在该体系中,·OH、SO_(4)·^(-)、1O2均参与了CTC的降解,贡献度最高的是1O2,其次为·OH和SO_(4)·^(-);基于反应前后XPS光谱对比分析,发现MnFeCu-LDHs活化PMS过程稳定性较好,此外该催化剂在重复使用5次后,CTC的30 min去除率仍达到73.61%。因此,本研究可为SR-AOPs应用于控制水环境抗生素类污染提供新思路。
Aiming at frequent detection of biorefractory organics,such as antibiotics in the tail water of wastewater treatment plant,MnFeCu layered double hydroxide (MnFeCu-LDHs) was prepared with green and low toxic transition metals to activate persulfate (PMS) for degrading chlortetracycline (CTC).The effects of initial pH,reaction temperature,catalyst and PMS dosage on CTC degradation efficiency were investigated.The types and contributions of reactive oxygen species (ROS) were determined through chemical capture and quenching experiments.The physicochemical properties of catalysts before and after reaction were characterized to investigate the stability of catalysts.The results showed that the removal rate of CTC reached 80.88% after 5min reaction,and 91.18% after 30 min reaction when the initial pH was 7,the reaction temperature was 298 K,and the dosages of catalyst and PMS were 0.2 g·L^(-1).Meanwhile,with the increase of initial pH and temperature,the degradation effect of CTC increased significantly.ROS quenching experiment and EPR capture confirmed that·OH,SO_(4)·^(-)and ~1O2participated in CTC degradation in this system,of which the highest contribution was ~1O2,followed by·OH and SO_(4)·-.Based on the comparative analysis results of XPS spectra before and after the reaction,it was found that the stability of MnFeCu-LDHs activated PMS process was reliable.In addition,after five recycles of the catalyst,the CTC degradation rate still reached 73.61% at 30 min reaction.Therefore,this study would provide a new insight for the application of SR-AOPs to control antibiotic pollution in water environment.
作者
朱建宇
党清平
杨帆
李军
吴嘉平
田亚军
ZHU Jianyu;DANG Qingping;YANG Fan;LI Jun;WU Jiaping;TIAN Yajun(Ocean College,Zhejiang University,Zhoushan 316021,China;North China Municipal Engineering Design and Research Institute Co.Ltd.,Tianjin 300074,China;College of Environment,Zhejiang University of Technology,Hangzhou 310014,China)
出处
《环境工程学报》
CAS
CSCD
北大核心
2022年第12期3895-3905,共11页
Chinese Journal of Environmental Engineering
基金
浙江省自然科学基金资助项目(LQ22E080027)
国家自然科学基金资助项目(42107411)。
