Mesoporous manganese Cobaltite nanocages as effective and reusable heterogeneous peroxymonosulfate activators for Carbamazepine degradation

被引:192
作者
Deng, Jing [1 ]
Cheng, Yong-qing [1 ]
Lu, Yu-an [1 ]
Crittenden, John C. [3 ,4 ]
Zhou, Shi-qing [5 ]
Gao, Nai-yun [6 ]
Li, Jun [2 ]
机构
[1] Zhejiang Univ Technol, Coll Civil Engn & Architecture, Hangzhou 310014, Zhejiang, Peoples R China
[2] Zhejiang Univ Technol, Coll Environm, Hangzhou 310014, Zhejiang, Peoples R China
[3] Georgia Inst Technol, Brook Byer Inst Sustainable Syst, Atlanta, GA 30332 USA
[4] Georgia Inst Technol, Sch Civil & Environm Engn, Atlanta, GA 30332 USA
[5] Hunan Univ, Dept Water Engn & Sci, Coll Civil Engn, Changsha 410082, Hunan, Peoples R China
[6] Tongji Univ, State Key Lab Pollut Control & Resource Reuse, Shanghai 200092, Peoples R China
基金
中国博士后科学基金; 中国国家自然科学基金;
关键词
Pharmaceutical residues; Carbamazepine (CBZ); MnxCo3 - O-x(4) nanocages; Peroxymonosulfate (PMS); Sulfate radical (SO4 (-center dot)); Degradation; ANTIEPILEPTIC DRUG CARBAMAZEPINE; METAL-ORGANIC FRAMEWORKS; EFFICIENT DEGRADATION; ADVANCED OXIDATION; BISPHENOL-A; PHOTOCATALYTIC DEGRADATION; CATALYTIC-OXIDATION; TREATMENT PLANTS; WATER; PERFORMANCE;
D O I
10.1016/j.cej.2017.07.149
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Mesoporous MnxCo3 - O-x(4) nanocages with high cobalt content, large surface area and high pore volume were synthesized through a self-assembly method. The as-prepared MnxCo3 - O-x(4) nanocages displayed satisfactory catalytic activity toward peroxymonosulfate (PMS) and the metal ions leaching concentration could be negligible. Sulfate radical was identified as the predominant active species through radical quenching experiments and electron spin resonance spin-trapping technique. The kinetics of the oxidation process was of pseudo-first order. The increasing cobalt content in MnxCo3 - O-x(4) NCs was in favor of enhancing the decomposition of PMS. MnxCo3 - O-x(4) nanocages dosage, PMS concentration and reaction temperature put the promoting effect on the degradation, while initial CBZ concentration had the retarding impact. MnxCo3 - O-x(4) nanocages could efficiently operate over a wide pH range of 5.0-8.0. Coexisting chloride ions exerted a dual role in the decomposition of PMS and this role was concentration-dependent. XPS analysis confirmed the reversible valence equilibrium between metal ions and the recovery of surface adsorbed oxygen, which ensured their sustainable catalytic activity even after five consecutive runs. Based on the main intermediates identified by liquid chromatography-tandem mass spectrometry, a possible pathway of CBZ oxidation was proposed. The potential risk resulting from the highly toxic intermediates can also be effectively controlled by MnxCo3 - O-x(4) NCs activated PMS system.
引用
收藏
页码:505 / 517
页数:13
相关论文
共 69 条
[1]   Solar photo-Fenton like using persulphate for carbamazepine removal from domestic wastewater [J].
Ahmed, Moussa Mahdi ;
Chiron, Serge .
WATER RESEARCH, 2014, 48 :229-236
[2]   Photocatalytic degradation of p-chlorophenol by hybrid H2O2 and TiO2 in aqueous suspensions under UV irradiation [J].
Anh Thu Nguyen ;
Juang, Ruey-Shin .
JOURNAL OF ENVIRONMENTAL MANAGEMENT, 2015, 147 :271-277
[3]   Chemical and microbial decontamination of pool water using activated potassium peroxymonosulfate [J].
Anipsitakis, George P. ;
Tufano, Thomas P. ;
Dionysiou, Dionysios D. .
WATER RESEARCH, 2008, 42 (12) :2899-2910
[4]   Transition metal/UV-based advanced oxidation technologies for water decontamination [J].
Anipsitakis, GP ;
Dionysiou, DD .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2004, 54 (03) :155-163
[5]   Heterogeneous activation of oxone using Co3O4 [J].
Anipsitakis, GP ;
Stathatos, E ;
Dionysiou, DD .
JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (27) :13052-13055
[6]   Radical generation by the interaction of transition metals with common oxidants [J].
Anipsitakis, GP ;
Dionysiou, DD .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2004, 38 (13) :3705-3712
[7]  
Atkins P., 2009, SHRIVER ATKINS INORG
[8]   Carbamazepine and its metabolites in wastewater: Analytical pitfalls and occurrence in Germany and Portugal [J].
Bahlmann, Arnold ;
Brack, Werner ;
Schneider, Rudolf J. ;
Krauss, Martin .
WATER RESEARCH, 2014, 57 :104-114
[9]   Ultrasound enhanced heterogeneous activation of peroxymonosulfate by a bimetallic Fe-Co/SBA-15 catalyst for the degradation of Orange II in water [J].
Cai, Chun ;
Zhang, Hui ;
Zhong, Xing ;
Hou, Liwei .
JOURNAL OF HAZARDOUS MATERIALS, 2015, 283 :70-79
[10]   Direct photodegradation of carbamazepine followed by micellar electrokinetic chromatography and mass spectrometry [J].
Calisto, Vania ;
Domingues, M. Rosario M. ;
Erny, Guillaume L. ;
Esteves, Valdemar I. .
WATER RESEARCH, 2011, 45 (03) :1095-1104