Synergistic catalytic degradation of antibiotic sulfamethazine in a heterogeneous sonophotolytic goethite/oxalate Fenton-like system

被引:98
作者
Zhou, Tao [1 ]
Wu, Xiaohui [1 ]
Zhang, Yanrong [1 ]
Li, Jianfeng [2 ]
Lim, Teik-Thye [3 ,4 ]
机构
[1] Huazhong Univ Sci & Technol, Sch Environm Sci & Engn, Wuhan 430074, Peoples R China
[2] Nanyang Technol Univ, Inst Environm Sci & Engn, Singapore 639732, Singapore
[3] Nanyang Technol Univ, Sch Civil & Environm Engn, Singapore 639798, Singapore
[4] Nanyang Technol Univ, NEWRI, Singapore 637141, Singapore
基金
新加坡国家研究基金会;
关键词
Sonophotocatalysis; Fenton-like; Sulfamethazine; Iron-oxalate complexes; Goethite; ADVANCED OXIDATION PROCESSES; 2,4-DICHLOROPHENOXYACETIC ACID; AQUATIC ENVIRONMENT; HYDROXYL RADICALS; ATMOSPHERIC WATER; HYDROGEN-PEROXIDE; AQUEOUS-SOLUTION; ORGANIC-LIGANDS; IRON-OXIDES; NEUTRAL PH;
D O I
10.1016/j.apcatb.2013.02.004
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
A novel heterogeneous sonophotolytic goethite/oxalate Fenton-like (SP-FL) system was developed in this study. Compared to the corresponding photochemical Fenton-like (P-FL) system and sonochemical Fenton-like system (S-FL) system, it was found that the SP-FL system could achieve synergistic degradation of antibiotic sulfamethazine (SMZ). A synergy factor of 2.2 based on pseudo-first-order degradation rate constant (k(obs)) was observed, along with great improvements in organic mineralization and waste-water detoxification. Examining the evolution of dissolved iron species and reactive oxygen species (H2O2 and center dot OH) in the three systems revealed that the SMZ degradation strongly relied on the "in-situ" photochemical generation of H2O2 and fast regeneration of dissolved Fe(II) species. Identification of the organic intermediates and released inorganic ions suggested that the cleavage of S-N bond in the SMZ molecule was dominant under center dot OH attacking. The important synergistic role of ultrasound (US) in promoting SMZ degradation was proposed. Herein US could affect the system at multi-folds: (1) accelerating the goethite-chelating dissolution by reducing mass transfer barriers, (2) enhancing the radical reactions in the bulk solution with sonochemical cavitation effect, and (3) possible direct hydrolysis of amine intermediates inside the cavitation bubbles. (C) 2013 Elsevier B.V. All rights reserved.
引用
收藏
页码:294 / 301
页数:8
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