Mn-MOF derived manganese sulfide as peroxymonosulfate activator for levofloxacin degradation: An electron-transfer dominated and radical/nonradical coupling process

被引:16
|
作者
Han, Xiaolin [1 ,2 ]
Zhang, Wei [1 ,2 ,3 ]
Li, Shuai [1 ,2 ]
Cheng, Congyu [1 ,2 ]
Yu, Qi [1 ]
Jia, Qilong [1 ,2 ]
Zhou, Lei [1 ,2 ,3 ]
Xiu, Guangli [1 ,2 ,3 ]
机构
[1] East China Univ Sci & Technol, Sch Resources & Environm Engn, State Environm Protect Key Lab Environm Risk Asses, Shanghai 200237, Peoples R China
[2] East China Univ Sci & Technol, Shanghai Environm Protect Key Lab Environm Stand &, Shanghai 200237, Peoples R China
[3] Tongji Univ, Shanghai Inst Pollut Control & Ecol Secur, Shanghai 200092, Peoples R China
来源
基金
中国国家自然科学基金; 上海市自然科学基金;
关键词
MnS; Metal organic frameworks; PMS; Levofloxacin; Electron-transfer pathway; BISPHENOL-A; SINGLET OXYGEN; OXIDATIVE-DEGRADATION; FACILE SYNTHESIS; ALPHA-MNS; PERSULFATE; GENERATION; MECHANISM; NANOPARTICLES; SUPEROXIDE;
D O I
10.1016/j.jes.2022.10.026
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Recently, transition metal sulfides have attracted much attention due to their better catalytic capacities as peroxymonosulfate (PMS) activator than their metal oxide counterparts. How-ever, the systematic studies on PMS activation using transition metal sulfides are still lack-ing. In this work, manganese sulfide (MnS) materials were synthesized via a MOFs-derived method and utilized for PMS activation to degrade levofloxacin (LVF) in water for the first time. As expected, MnS exhibited remarkable LVF degradation efficiency by PMS activation, which was distinctly higher than Mn2O3. The results of quenching experiments, electro spin resonance identification and electrochemical tests indicated that electron-transfer progress was the dominant mechanism in a-MnS/PMS system. Meanwhile, the presence of 1 O 2 and radicals further became the removal of LVF by a-MnS/PMS system into a radical/nonradical coupling process. The superior electrical conductivity of a-MnS than a-Mn2O3 was revealed by DFT calculations, which resulted in the higher catalytic capacity of a-MnS. The result of XPS also indicated the S species in MnS accelerated the recycle of Mn(IV)/Mn(II) and then promoted the generation of radicals. Furthermore, the influence of various environmen-tal conditions on LVF removal and the reusability of a-MnS were also investigated, which demonstrated the high application potential of a-MnS/PMS system. Finally, six possible pathways of LVF oxidation in the system were proposed based on the identified byproducts
引用
收藏
页码:197 / 211
页数:15
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