Citrate-regulated synthesis of hydrotalcite-like compounds as peroxymonosulfate activator - Investigation of oxygen vacancies and degradation pathways by combining DFT

被引:141
作者
Qin, Lei [1 ,2 ]
Ye, Haoyang [1 ,2 ]
Lai, Cui [1 ,2 ]
Liu, Shiyu [1 ,2 ]
Zhou, Xuerong [1 ,2 ]
Qin, Fanzhi [1 ,2 ]
Ma, Dengsheng [1 ,2 ]
Long, Baoyu [1 ,2 ]
Sun, Yuyan [1 ,2 ]
Tang, Lin [1 ,2 ]
Yan, Ming [1 ,2 ]
Chen, Wenfang [1 ,2 ]
Chen, Wenjing [1 ,2 ]
Xiang, Ling [1 ,2 ]
机构
[1] Hunan Univ, Coll Environm Sci & Engn, Changsha 410082, Peoples R China
[2] Hunan Univ, Key Lab Environm Biol & Pollut Control, Minist Educ, Changsha 410082, Peoples R China
来源
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY | 2022年 / 317卷
基金
中国国家自然科学基金; 湖南省自然科学基金;
关键词
Antibiotic; Hydrotalcite-like compounds; Oxygen vacancy regulation strategies; Peroxymonosulfate activation; Theoretical chemical calculation; LAYERED DOUBLE HYDROXIDES; WASTE-WATER TREATMENT; EFFICIENT DEGRADATION; ADVANCED OXIDATION; UREA HYDROLYSIS; RATE CONSTANTS; REMOVAL; LDH; MORPHOLOGY; CIPROFLOXACIN;
D O I
10.1016/j.apcatb.2022.121704
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
This work investigated the triggering mechanism of peroxymonosulfate (PMS) activated by an oxygen vacancy (Ov)-rich cobalt (Co)-based hydrotalcite-like compound (CA-LDH). CA-LDH was synthesized by a urea -hydrothermal process with ammonium citrate (CA) as the reducing agent. The PMS activation mechanism was investigated by combining batch experiments, characterization techniques, and DFT calculations. Over 98 % of CIP (20 mg/L) was degraded by the CA-LDH/PMS system within 60 min, which remained efficient in the presence of common interfering substances or over a wide pH range. DFT showed that CA was beneficial for introducing the electron transfer intermediate, namely, O-v, on CA-LDH, thereby allowing for the unique electron transfer performance of CA-LDH. Specifically, electron transfer from Co-O-v to PMS triggered the radical pathway, while electron transfer from PMS to Co-O-v triggered the nonradical pathway. Overall, this study provides a reference for the rational catalyst synthesis and the investigation of the triggering mechanism of PMS activation.
引用
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页数:14
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