Heterogeneous activation of peroxymonosulfate by LaFeO3 for diclofenac degradation: DFT-assisted mechanistic study and degradation pathways | |
Rao, YongFang1,5; Zhang, Yufei2,3; Han, Fuman1; Guo, Huichao1; Huang, Yu2,3; Li, Ruoyu4; Qi, Fei4; Ma, Jun5 | |
2018-11-15 | |
发表期刊 | CHEMICAL ENGINEERING JOURNAL |
卷号 | 352页码:601-611 |
文章类型 | Article |
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 | Lafeo3 Peroxylmonosulfate (Pms) Diclofenac (Dcf) Dft Reaction Mechanisms Degradation Pathways |
WOS标题词 | Science & Technology ; Technology |
DOI | 10.1016/j.cej.2018.07.062 |
关键词[WOS] | ANTIINFLAMMATORY DRUG DICLOFENAC ; AQUEOUS-SOLUTION ; SULFATE RADICALS ; RATE CONSTANTS ; ADVANCED OXIDATION ; TREATMENT PLANTS ; NO REMOVAL ; PEROVSKITE ; CATALYSTS ; WATER |
收录类别 | SCI |
语种 | 英语 |
WOS研究方向 | Engineering |
WOS类目 | Engineering, Environmental ; Engineering, Chemical |
WOS记录号 | WOS:000444001900065 |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://ir.ieecas.cn/handle/361006/5344 |
专题 | 粉尘与环境研究室 |
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 |
推荐引用方式 GB/T 7714 | 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. |
APA | Rao, YongFang.,Zhang, Yufei.,Han, Fuman.,Guo, Huichao.,Huang, Yu.,...&Ma, Jun.(2018).Heterogeneous activation of peroxymonosulfate by LaFeO3 for diclofenac degradation: DFT-assisted mechanistic study and degradation pathways.CHEMICAL ENGINEERING JOURNAL,352,601-611. |
MLA | Rao, YongFang,et al."Heterogeneous activation of peroxymonosulfate by LaFeO3 for diclofenac degradation: DFT-assisted mechanistic study and degradation pathways".CHEMICAL ENGINEERING JOURNAL 352(2018):601-611. |
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