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题名: Heterogeneous activation of peroxymonosulfate by LaFeO3 for diclofenac degradation: DFT-assisted mechanistic study and degradation pathways
作者: Rao, YongFang1, 5;  Zhang, Yufei2, 3;  Han, Fuman1;  Guo, Huichao1;  Huang, Yu2, 3;  Li, Ruoyu4;  Qi, Fei4;  Ma, Jun5
关键词: LaFeO3 ;  Peroxylmonosulfate (PMS) ;  Diclofenac (DCF) ;  DFT ;  Reaction mechanisms ;  Degradation pathways
刊名: CHEMICAL ENGINEERING JOURNAL
发表日期: 2018-11-15
DOI: 10.1016/j.cej.2018.07.062
卷: 352, 页:601-611
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Technology
类目[WOS]: Engineering, Environmental ;  Engineering, Chemical
研究领域[WOS]: Engineering
英文摘要: A perovskite oxide, LaFeO3 (LFO), was synthesized and evaluated as a heterogeneous catalyst to activate peroxymonosulfate (PMS) for the oxidative degradation of diclofenac (DCF), a non-steroidal anti-inflammatory drug. It was observed that the catalytic activity of LFO was much higher than that of Fe2O3. LFO catalyzed PMS to degrade DCF with a turnover frequency (2.02 x 10(-3) min(-1))which is 17-fold higher than that of Fe2O3. Both sulfate and hydroxyl radicals were identified during LFO-activated PMS process by electron spin resonance (ESR). Radical competitive reactions indicate sulfate radicals played a major role in DCF degradation by LFO/PMS process. The PMS decomposition can be attributed to the formation of an inner-sphere complexation between the Fe (III) sites on LFO surface and PMS. Theoretical calculations illustrated the strong interaction between PMS and Fe (III) and electron transfer from PMS to Fe (III). Hydrogen temperature-programmed reduction (H-2-TPR) indicates that the LFO perovskite oxide is capable of facilitating an easier reduction of Fe (III) to mediate a redox process. Oxygen temperature-programmed desorption (O-2-TPD) suggests much more oxygen vacancies exist in LFO than in Fe2O3. Oxygen vacancies are favorable for the formation of chemical bond between Fe (III) and PMS and the activation of PMS. In situ ATR-FTIR analysis of LFO surface during PMS decomposition implies Fe (III)-Fe(II)-Fe (III) redox cycle was believed to account for the generation of sulfate radical. The intermediates generated during DCF degradation were identified and the possible degradation pathways were advanced in LFO/PMS system.
关键词[WOS]: ANTIINFLAMMATORY DRUG DICLOFENAC ;  AQUEOUS-SOLUTION ;  SULFATE RADICALS ;  RATE CONSTANTS ;  ADVANCED OXIDATION ;  TREATMENT PLANTS ;  NO REMOVAL ;  PEROVSKITE ;  CATALYSTS ;  WATER
语种: 英语
WOS记录号: WOS:000444001900065
Citation statistics: 
内容类型: 期刊论文
URI标识: http://ir.ieecas.cn/handle/361006/5344
Appears in Collections:粉尘与环境研究室_期刊论文

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作者单位: 1.Xi An Jiao Tong Univ, Dept Environm Sci & Engn, Xian 710049, Shaanxi, Peoples R China
2.Chinese Acad Sci, Inst Earth Environm, Key Lab Aerosol Chem & Phys, Xian 710075, Shaanxi, Peoples R China
3.Chinese Acad Sci, Inst Earth Environm, SKLLQG, Xian 710075, Shaanxi, Peoples R China
4.Beijing Forestry Univ, Coll Environm Sci & Engn, Beijing 100083, Peoples R China
5.Harbin Inst Technol, State Key Lab Urban Water Resource & Environm, Harbin 150090, Heilongjiang, Peoples R China

Recommended Citation:
Rao, YongFang,Zhang, Yufei,Han, Fuman,et al. Heterogeneous activation of peroxymonosulfate by LaFeO3 for diclofenac degradation: DFT-assisted mechanistic study and degradation pathways[J]. CHEMICAL ENGINEERING JOURNAL,2018,352:601-611.
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