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Efficient Removal of Antibiotic Resistance Genes through 4f-2p-3d Gradient Orbital Coupling Mediated Fenton-Like Redox Processes |
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| Authors: | Fei Li Pengfei Wang Tao Zhang Mingmei Li Shuai Yue Prof. Sihui Zhan Prof. Yi Li |
| Affiliation: | 1. MOE 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 Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin University, 300072 Tianjin, P. R. China These authors contributed equally to this work.;2. MOE 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 These authors contributed equally to this work.;3. MOE 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;4. Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin University, 300072 Tianjin, P. R. China |
| Abstract: | Peroxymonosulfate (PMS) mediated radical and nonradical active substances can synergistically achieve the efficient elimination of antibiotic resistance genes (ARGs). However, enhancing interface electron cycling and optimizing the coupling of the oxygen-containing intermediates to improve PMS activation kinetics remains a major challenge. Here, Co doped CeVO4 catalyst (Co−CVO) with asymmetric sites was constructed based on Ce 4f−O 2p−Co 3d gradient orbital coupling. The catalyst achieved approximately 2.51×105 copies/mL of extracellular ARGs (eARGs) removal within 15 minutes, exhibited ultrahigh degradation rate (k=1.24 min−1). The effective gradient 4f-2p-3d orbital coupling precisely regulates the electron distribution of Ce−O−Co active center microenvironment, while optimizing the electronic structure of Co 3d states (especially the occupancy of eg), promoting the adsorption of oxygen-containing intermediates. The generated radical and nonradical generated by interfacial electron cycling enhanced by the reduction reaction of PMS at the Ce site and the oxidation reaction at the Co site achieved a significant mineralization rate of ARGs (83.4 %). The efficient removal of ARGs by a continuous flow reactor for 10 hours significantly reduces the ecological risk of ARGs in actual wastewater treatment. |
| Keywords: | Antibiotic Resistance Genes Asymmetric Sites Gradient Orbital Coupling PMS Activation |