How metal/support interaction improved degradation performance in the peroxymonosulfate activation process: significance of high-valent cobalt-oxo species

被引:0
|
作者
Fan, Xing [1 ,2 ,3 ]
Zhang, Wei [1 ,2 ,3 ]
Yan, Huchuan [1 ,2 ,3 ]
Lai, Cui [1 ,2 ,3 ]
Ma, Dengsheng [1 ,2 ]
Liu, Shiyu [1 ,2 ,3 ]
Zhang, Mingming [1 ,2 ,3 ]
Li, Ling [1 ,2 ,3 ]
Zhou, Xuerong [1 ,2 ,3 ]
Huo, Xiuqin [1 ,2 ,3 ]
Xu, Fuhang [1 ,2 ,3 ]
Hu, Xiaorui [1 ,2 ]
Wang, Biting [1 ,2 ]
Sun, Hao [1 ,2 ]
He, Wuqiang [4 ]
机构
[1] Hunan Univ, Coll Environm Sci & Engn, Changsha 410082, Hunan, Peoples R China
[2] Hunan Univ, Key Lab Environm Biol & Pollut Control, Minist Educ, Changsha 410082, Peoples R China
[3] Hunan Univ Chongqing, Res Inst, Chongqing 401120, Peoples R China
[4] Hunan Univ Technol, Coll Mat & Adv Mfg, Zhuzhou 412007, Peoples R China
基金
湖南省自然科学基金; 中国国家自然科学基金;
关键词
ELECTRONIC-STRUCTURE; OXIDATION; CATALYST; WATER;
D O I
10.1039/d4en00355a
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Currently, the strategy of metal loading is expected to promote the nonradical catalytic activity of transition metal spinel oxide catalysts in peroxymonosulfate (PMS) systems, but the connection between the mechanism of degradation performance improvement and metal-support interaction (MSI) remains unclear. Herein, a novel CoFe2O4 loaded sepiolite composite (10-CFS) was prepared for PMS activation to degrade ciprofloxacin (CIP). 10-CFS exhibited outstanding PMS activation ability, and 98.7% of CIP was degraded within 30 min, which was significantly higher than that of the physical mixture of sepiolite and CoFe2O4 (59.8%). A series of experiments demonstrated that the presence of Co(iv) 00000000 00000000 00000000 00000000 11111111 00000000 11111111 00000000 00000000 00000000 O caused the better degradation performance of 10-CFS. Notably, theoretical calculations signified that MSI not only promoted the coupled electron-proton transfer (CEPT) process and thus changed the formation pathway of Co(iv)O, but also facilitated PMS adsorption on 10-CFS and lowered the energy barrier for Co(iv)O generation. In summary, this study illustrates deeply the mechanism of catalytic performance improvement after metal loading by focusing on the MSI and bridges the gap in understanding the MSI and degradation performance. 10-CFS exhibited outstanding PMS activation ability, 98.7% of CIP was degraded within 30 min. The result demonstrated that the presence of Co(iv)O caused the better degradation performance of 10-CFS.
引用
收藏
页码:4754 / 4764
页数:11
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