Degradation of sulfamethoxazole by Co3O4-palygorskite composites activated peroxymonosulfate oxidation

被引:89
作者
Yu, Yaqun [1 ]
Ji, Yuefei [1 ]
Lu, Junhe [1 ]
Yin, Xiaoming [1 ]
Zhou, Quansuo [1 ]
机构
[1] Nanjing Agr Univ, Dept Environm Sci & Engn, Nanjing 210095, Peoples R China
基金
中国国家自然科学基金;
关键词
Co3O4-palygorskite; Peroxymonosulfate; Sulfate radical; Sulfamethoxazole; Reaction mechanisms; Transformation pathways; PERSULFATE OXIDATION; ORGANIC POLLUTANTS; GRAPHENE OXIDE; RATE CONSTANTS; ORANGE II; WATER; KINETICS; PHARMACEUTICALS; NANOPARTICLES; MECHANISM;
D O I
10.1016/j.cej.2020.126759
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
In this study, a simple hydrothermal method was used to synthesize Co3O4-palygorskite composites. Transmission electron microscopy, X-ray spectroscopy and X-ray diffraction analysis showed that Co3O4 nanoparticles with diameters of approximately 3-5 nm were uniformly distributed on the surface of palygorskite fibers. Co3O4-palygorskite composites were outstanding catalyst for activating peroxymonosulfate (PMS) to degrade the antibiotic sulfamethoxazole (SMX). Complete removal of 30 mu M SMX at pH 3-5 was achieved with doses of 0.3 mM PMS and 125 mg/L Co3O4-palygorskite composites. The composites exhibited higher catalytical activity than unsupported Co3O4. The removal rate of SMX was accelerated under acidic conditions (pH 3-5), while was significantly inhibited under basic conditions (pH 11-12). Radical quenching tests revealed that SO4 center dot- and center dot OH were responsible for the degradation. The oxidative degradation was initiated at either isoxazole or aniline moiety of the SMX molecule. Using solid phase extraction-liquid chromatography-time-of-flight-tandem mass spectrometry, a total of six transformation products formed from benzene ring hydroxylation, S-N bond cleavage, aniline moiety oxidation and coupling reactions were identified. Based on the products, three transformation pathways are proposed for the catalytic degradation of SMX in the Co3O4-palygorskite/PMS system.
引用
收藏
页数:12
相关论文
共 67 条
[1]   Sulfate radical anion oxidation of diclofenac and sulfamethoxazole for water decontamination [J].
Ahmed, Moussa Mahdi ;
Barbati, Stephane ;
Doumenq, Pierre ;
Chiron, Serge .
CHEMICAL ENGINEERING JOURNAL, 2012, 197 :440-447
[2]   Degradation of organic contaminants in water with sulfate radicals generated by the conjunction of peroxymonosulfate with cobalt [J].
Anipsitakis, GP ;
Dionysiou, DD .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2003, 37 (20) :4790-4797
[3]   Cobalt-mediated activation of peroxymonosulfate and sulfate radical attack on phenolic compounds. Implications of chloride ions [J].
Anipsitakis, GP ;
Dionysiou, DD ;
Gonzalez, MA .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2006, 40 (03) :1000-1007
[4]   Radical generation by the interaction of transition metals with common oxidants [J].
Anipsitakis, GP ;
Dionysiou, DD .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2004, 38 (13) :3705-3712
[5]  
ANNE LB, 2004, ENVIRON SCI TECHNOL, V38, P3933
[6]   Potentiometric mass titrations: Experimental and theoretical establishment of a new technique for determining the point of zero charge (PZC) of metal (hydr)oxides [J].
Bourikas, K ;
Vakros, J ;
Kordulis, C ;
Lycourghiotis, A .
JOURNAL OF PHYSICAL CHEMISTRY B, 2003, 107 (35) :9441-9451
[7]   CRITICAL-REVIEW OF RATE CONSTANTS FOR REACTIONS OF HYDRATED ELECTRONS, HYDROGEN-ATOMS AND HYDROXYL RADICALS (.OH/.O-) IN AQUEOUS-SOLUTION [J].
BUXTON, GV ;
GREENSTOCK, CL ;
HELMAN, WP ;
ROSS, AB .
JOURNAL OF PHYSICAL AND CHEMICAL REFERENCE DATA, 1988, 17 (02) :513-886
[8]   Inhibitory effect of dissolved organic matter on triplet-induced oxidation of aquatic contaminants [J].
Canonica, Silvio ;
Laubscher, Hans-Ulrich .
PHOTOCHEMICAL & PHOTOBIOLOGICAL SCIENCES, 2008, 7 (05) :547-551
[9]   Overview of sulfonamide biodegradation and the relevant pathways and microorganisms [J].
Chen, Jianfei ;
Xie, Shuguang .
SCIENCE OF THE TOTAL ENVIRONMENT, 2018, 640 :1465-1477
[10]   Mesoporous bouquet-like Co3O4 nanostructure for the effective heterogeneous activation of peroxymonosulfate [J].
Chen, Liwei ;
Cai, Tianming ;
Sun, Wenjie ;
Zuo, Xu ;
Ding, Dahu .
JOURNAL OF THE TAIWAN INSTITUTE OF CHEMICAL ENGINEERS, 2017, 80 :720-727