Qin Jiani, Duan Minna, Zhang Yi, Hua Ruochen, Zhang Yongqi, Wang Chuanyi, Pan Bao
School of Environmental Science and Engineering, Shaanxi University of Science and Technology, Xi'an 710021, P. R. China.
School of Environmental Science and Engineering, Shaanxi University of Science and Technology, Xi'an 710021, P. R. China; Department of Environmental and Sustainable Engineering, Faculty of Engineering, Chulalongkorn University, 254 Phayathai Road, Pathumwan, Bangkok, 10330, Thailand.
Environ Res. 2025 Jul 29:122460. doi: 10.1016/j.envres.2025.122460.
The widespread use of tetracycline (TC) antibiotics poses significant environmental and health risks due to their persistence and toxicity in aquatic ecosystems. In this study, a heterogeneous catalyst composed of CoO supported on graphitic carbon nitride (CoO/CN) was developed to efficiently activate peroxymonosulfate (PMS) for TC degradation. A series of CoO/CN composites with different cobalt loadings were synthesized via a straightforward pyrolysis process. The optimized 12%CoO/CN sample exhibited an enhanced specific surface area, abundant nitrogen vacancies, and improved electron transfer efficiency, achieving 86.6% degradation of TC within 30 min, with 5.4-fold enhancement in reaction rate constant than PMS-only systems. Consistently high degradation efficiencies were also observed for various other micropollutants. Mechanism investigations revealed that O· radicals played a dominant role in TC degradation, while SO·, O, and ·OH radicals also contributed significantly, all synergistically promoted by the redox cycling of Co/Co species and the presence of nitrogen vacancies. Notably, the catalytic system exhibited broad pH adaptability, excellent reusability, and effective mineralization capacity. Toxicity assessment further indicated a reduced ecotoxicity of TC degradation byproducts. This study thus offers a promising and environmentally sustainable solution for the effective remediation of antibiotic-contaminated wastewater.
四环素（TC）类抗生素的广泛使用因其在水生生态系统中的持久性和毒性而带来了重大的环境和健康风险。在本研究中，开发了一种由负载在石墨相氮化碳上的CoO组成的非均相催化剂（CoO/CN），用于高效活化过一硫酸盐（PMS）以降解TC。通过简单的热解过程合成了一系列具有不同钴负载量的CoO/CN复合材料。优化后的12%CoO/CN样品具有更大的比表面积、丰富的氮空位和更高的电子转移效率，在30分钟内实现了86.6%的TC降解，反应速率常数比仅使用PMS的系统提高了5.4倍。对于各种其他微污染物也观察到了持续较高的降解效率。机理研究表明，O·自由基在TC降解中起主导作用，而SO·、O和·OH自由基也有显著贡献，所有这些都通过Co/Co物种的氧化还原循环和氮空位的存在协同促进。值得注意的是，该催化系统表现出广泛的pH适应性、优异的可重复使用性和有效的矿化能力。毒性评估进一步表明TC降解副产物的生态毒性降低。因此，本研究为有效修复抗生素污染废水提供了一种有前景且环境可持续的解决方案。
