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通过4f-2p-3d梯度轨道合介导的芬顿式氧化过程有效地去除抗生素耐药性基因

Fei Li^1,2, Pengfei Wang¹, Tao Zhang¹

¹MOE Key Laboratory of Pollution Processes and Environmental Criteria, Tianjin Key Laboratory of Environmental Remediation and Pollution Control, College of Environmental Science and Engineering, Nankai University, 300350, Tianjin, P. R. China.

Angewandte Chemie (International ed. in English)

|October 5, 2023

概括

这项研究引入了一种新型的-化瓦纳酸盐催化剂 (Co-CVO),用于有效地从水中去除抗生素耐药性基因 (ARG). 催化剂利用轨道合激活氧硫酸盐 (PMS),实现快速和完整的ARG降解.

科学领域:

环境化学环境化学
材料科学材料科学材料科学
催化剂是一种催化剂.

背景情况:

抗生素耐药性基因 (ARG) 构成重大环境和健康风险.
氧硫酸盐 (PMS) 激活对于降解ARG至关重要,但在增强电子循环和中间合方面仍然存在挑战.
开发用于PMS激活的有效催化剂对于有效的废水处理至关重要.

研究的目的:

构建一种新型的化瓦纳酸盐 (Co-CVO) 催化剂,具有不对称的位点,用于增强PMS激活.
研究由Co-CVO催化剂调解的PMS激活和ARG降解的机制.
评估催化剂在连续流条件下从废水中去除ARG的效率.

主要方法:

合成使用Ce 4f-O 2p-Co 3d梯度轨道合的联合合的CeVO4催化剂 (Co-CVO).
研究PMS激活动力学和在催化剂活性位点的电子转移通路.
对细胞外ARG (eARG) 清除效率和降解率的实验性评估.
对反应中间体和矿化速率的分析.
在连续流反应堆中测试催化剂,用于长期废水处理.

主要成果:

协同CVO催化剂证明了eARG的快速去除 (大约1. 2.51×10^5副本/毫升在15分钟内) 具有超高的降解率 (k=1.24分钟-1).
有效的梯度4f-2p-3d轨道合精确调节电子分布,优化Co 3d状态并促进含氧中间吸附.
通过界面电子循环 (Ce 减少,Co 氧化) 产生的协同激进和非激进物种实现了83.4%的ARG矿化.
连续10小时的流量处理显示了有效的ARG去除,减少了生态风险.

结论:

同-CVO催化剂通过梯度轨道合有效地激活PMS,增强电子循环和中间吸附,以降解高级ARG.
催化剂显示出在废水处理中实际应用的巨大潜力,以减轻与ARG相关的生态风险.

关键词:

抗生素耐药性基因抗生素耐药性基因不对称的网站梯度轨道合器梯度轨道合器预孕MS激活方式

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