Orientated construction of visible-light-assisted peroxymonosulfate activation system for antibiotic removal: Significant enhancing effect of Cl-
Orientated construction of visible-light-assisted peroxymonosulfate activation system for antibiotic removal: Significant enhancing effect of Cl-
复制标题
定向构建可见光辅助过一硫酸盐活化系统去除抗生素：Cl-显着增强作用
DOI：
10.1016/j.jhazmat.2022.130476
复制
发表时间：
2022
影响因子：
13.6
通讯作者：
Fei Chen
中科院分区：
文献类型：
--
作者：
Ke-An Zhu;Xin-Jia Chen;Chao-Wei Yuan;Chang-Wei Bai;Yi-Jiao Sun;Bin-Bin Zhang;Fei Chen
抗生素污染物可以在水中长距离迁移，从而可能对环境造成严重损害，甚至对人体健康造成潜在危害。可见光辅助下过氧单硫酸盐（PMS）的非均相活化是一种新兴的、有前途的废水净化技术。本研究设计了一种超高效稳定的PMS活化剂（FeCN），用于在恶劣条件下恢复典型的抗生素污染水。在构建的FeCN+PMS/vis体系中，35 min内磺胺甲恶唑（SMX）的降解率为90.94%，反应速率常数比直接光催化提高了近50倍。电子自旋共振、猝灭实验、LC/MS技术、生态毒性评价和密度泛函理论验证了SMX的去除以h+、•o2和2o对高福井指数SMX分子活性原子的攻击为主，呈现出降解和解毒同时进行的过程。这种可见光辅助的PMS活化体系对环境水体具有良好的抗性，对各种污染物的降解具有广谱性。其中Cl-(50 mM)能显著加速SMX的脱除，催化活性提高32.6倍，矿化效率达到56.6%。此外，这种含氯系统排除了消毒副产物的降解产物，并且这种系统对于不同的污染物也是通用的。这项工作证明了FeCN+PMS/vis系统在存在和不存在Cl-的情况下修复抗生素污染废水的可行性，并强调了它们在污水处理厂的巨大潜力。
Antibiotic contaminants can migrate over long distances in the water, thus possibly causing severe detriment to the environment and even potential harm to human health. Heterogeneous activation of peroxymonosulfate (PMS) assisted by visible light is an emerging and promising technology for the purification of such wastewater. This study designed an ultra-efficient and stable PMS activator (FeCN) to restore the typical antibiotic-polluted water under harsh conditions. About 90.94% of sulfamethoxazole (SMX) was degraded in 35 min in the constructed FeCN+PMS/vis system, and the reaction rate constant was nearly 50-fold higher than direct photocatalysis. Electron spin resonance, quenching experiments, LC/MS technique, eco-toxicity assessment, and density functional theory validated that the SMX removal was dominated by the attack of h+,•O2-and1O2on the active atoms of SMX molecules with high Fukui index, presenting as a simultaneous degradation and detoxification process. Such a visible-light-assisted PMS activation system also had good resistance to the environmental water bodies and a broad spectrum in the degradation of various pollutants. In particular, Cl-(50 mM) could significantly accelerate the removal of SMX with a 32.6-fold increase in catalytic activity, and the mineralization efficiency could reach 56.6% under identical conditions. Moreover, this Cl-containing system excluded the degradation products of disinfection by-products, and such a system was also versatile for different contaminants. This work demonstrates the feasibility of the FeCN+PMS/vis system for the remediation of antibiotic-contaminated wastewater in the presence and absence of Cl-, and also highlights their great potential in WWTPs.