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

石墨烯 降级(电信) 催化作用 激活剂(遗传学) 化学 化学工程 四环素 微波食品加热 碳纤维 材料科学 纳米技术 光化学 无机化学 有机化学 工程类 复合数 生物化学 复合材料 电信 抗生素 计算机科学 基因
作者
Lei Liu,Meiying Yu,Yunfei Li,Chunjiang Han,Guofang Ding,Shengnan Liu,Yunxuan Xie,Jia Liu
出处
期刊:Separation and Purification Technology [Elsevier BV]
卷期号:295: 121358-121358 被引量:26
标识
DOI:10.1016/j.seppur.2022.121358
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 ([email protected]) 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 [email protected] exhibited excellent dispersibility and catalytic performance. The [email protected]/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 Co3O4/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 1O2 served as the main contributor to TC degradation besides radicals (i.e., SO4−, OH, and O2−). Density functional theory (DFT) calculations unveiled the synergistic interaction of [email protected], 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.
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