Microwave (MW)-assisted design of cobalt anchored 2D graphene-like carbon nanosheets (Co@GCNs) as peroxymonosulfate activator for tetracycline degradation and insight into the catalytic mechanism

被引:25
作者
Liu, Lei [1 ]
Yu, Meiying [1 ]
Li, Yunfei [1 ]
Han, Chunjiang [1 ]
Ding, Guofang [1 ]
Liu, Shengnan [1 ]
Xie, Yunxuan [1 ]
Liu, Jia [1 ]
机构
[1] Tianjin Univ, Acad Environm & Ecol, Sch Environm Sci & Engn, 92 Weijin Rd, Tianjin 300072, Peoples R China
基金
国家重点研发计划;
关键词
Co@GCNs; Microwave-assisted; Peroxymonosulfate; Tetracycline; Non-radical pathway; CARE PRODUCTS PPCPS; EFFICIENT DEGRADATION; HETEROGENEOUS CATALYSIS; ORGANIC POLLUTANTS; OXIDATION PROCESS; SINGLET OXYGEN; BISPHENOL-A; PERFORMANCE; REMOVAL; PHARMACEUTICALS;
D O I
10.1016/j.seppur.2022.121358
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
Developing a rapid and cost-effective strategy to design catalysts for advanced oxidation processes (AOPs) has significant implications for environmental remediation. In this study, cobalt anchored 2D graphene-like carbon nanosheets (Co@GCNs) catalysts were fabricated by simple coordination of metal precursors into agarose through microwave (MW)-assisted method to activate peroxymonosulfate (PMS) for tetracycline (TC) degradation. Among them, the Co@GCN-1 exhibited excellent dispersibility and catalytic performance. The Co@GCN-1/ PMS system could completely degrade TC (20 mg L-1) within 20 min, whose reaction rate constant (0.273 min(-1)) was about 6.5 times that of the Co3O(4/)PMS system (0.0362 min(-1)) and 14.1 times of the GCN/PMS system (0.0194 min(-1)), respectively. Additionally, the degradation performance was applicable in a wide pH range (3.84-9.03) and still reached an efficiency of>90% after five cycles. Non-radical pathway represented by O-1(2) served as the main contributor to TC degradation besides radicals (i.e., SO4 center dot-, (OH)-O-center dot, and O-2(center dot-)). Density functional theory (DFT) calculations unveiled the synergistic interaction of Co@GCNs, where 2D GCNs as electron mediators promoted the Co3+/Co2+ cycle. Based on the LC-MS analysis, three main degradation pathways of TC including fourteen possible intermediates were proposed based on different ROS reactions. This work provides a facilely prepared and promising 2D metal-based carbonous catalyst to activate PMS for the efficient degradation of TC.
引用
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页数:15
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