Zhao Jiang, Chen Tianyin, Hou Cheng, Huang Baorong, Du Jiawen, Liu Nengqian, Zhou Xuefei, Zhang Yalei
State Key Laboratory of Pollution Control and Resources Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China.
Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China.
Nanomaterials (Basel). 2022 Aug 18;12(16):2842. doi: 10.3390/nano12162842.
The removal of contaminants of emerging concern (CECs) has become a hot research topic in the field of environmental engineering in recent years. In this work, a simple pyrolysis method was designed to prepare a high-performance biochar-loaded zero-valent copper (CuC) material for the catalytic degradation of antibiotics ENR by PMS. The results showed that 10 mg/L of ENR was completely removed within 30 min at an initial pH of 3, CuC 0.3 g/L, and PMS 2 mmol/L. Further studies confirmed that the reactive oxygen species (ROS) involved in ENR degradation are ·OH, SO4-·, O, and O2-. Among them, O played a major role in degradation, whereas O2-· played a key role in the indirect generation of O. On the one hand, CuC adsorbed and activated PMS to generate ·OH, SO4-· and O2-·. O2-· was unstable and reacted rapidly with HO and ·OH to generate large amounts of O. On the other hand, both the self-decomposition of PMS and direct activation of PMS by C=O on biochar also generated O. Five byproducts were generated during degradation and eventually mineralized to CO, HO, NO3-, and F. This study provides a facile strategy and new insights into the biochar-loaded zero-valent transition-metal-catalyzed PMS degradation of CECs.
近年来,去除新兴关注污染物(CECs)已成为环境工程领域的一个热门研究课题。在这项工作中,设计了一种简单的热解方法来制备一种高性能的负载生物炭的零价铜(CuC)材料,用于过一硫酸盐(PMS)催化降解抗生素恩诺沙星(ENR)。结果表明,在初始pH为3、CuC浓度为0.3 g/L和PMS浓度为2 mmol/L的条件下,10 mg/L的ENR在30分钟内被完全去除。进一步的研究证实,参与ENR降解的活性氧物种(ROS)为·OH、SO4-·、O和O2-·。其中,O在降解中起主要作用,而O2-·在O的间接生成中起关键作用。一方面,CuC吸附并活化PMS生成·OH、SO4-·和O2-·。O2-·不稳定,与HO和·OH迅速反应生成大量的O。另一方面,PMS的自分解以及生物炭上的C=O对PMS的直接活化也生成O。降解过程中产生了五种副产物,最终矿化为CO、HO、NO3-和F。本研究为负载生物炭的零价过渡金属催化PMS降解CECs提供了一种简便策略和新的见解。