Qian Jin, Zhang Yichu, Chen Zhijie, Yu Ran, Ye Yin, Ma Rui, Li Kailong, Wang Lingzhen, Wang Dongqi, Ni Bing-Jie
School of Chemistry and Chemical Engineering, Northwestern Polytechnical University, Xi'an, Shaanxi, 710072, China.
Centre for Technology in Water and Wastewater, School of Civil and Environmental Engineering, University of Technology Sydney, NSW, 2007, Australia.
J Environ Manage. 2023 Oct 15;344:118440. doi: 10.1016/j.jenvman.2023.118440. Epub 2023 Jun 19.
Peroxymonosulfate (PMS)-mediated advanced oxidation processes gain growing attention in degrading antibiotics (e.g., tetracycline (TC)) in wastewater for their high capacity and relatively low cost, while designing efficient catalysts for PMS activation remains a challenge. In this study, a sulfur-doped Fe/C catalyst (Fe@C-S) synthesized from iron metal-organic frameworks (Fe-MOFs) was developed for PMS activation towards TC removal. Under optimal conditions, the TC removal efficiency of Fe@C-S150/PMS system within 40 min was 91.2%. Meanwhile, the k value for Fe@C-S150/PMS system (0.2038 min) was 3.36-fold as high as the S-free Fe@C-based PMS system. Also, Fe@C-S150/PMS system showed high robustness in different water matrices. Further studies found that the TC degradation mechanism was mainly ascribed to the non-radical pathway (O and electron transfer). Fe nanoparticles, S and CO groups on the catalyst all participated in the generation of reactive oxygen species (ROS). Besides, S species could enhance the Fe/Fe redox cycle and accelerate the electron transfer process. This work highlights the critical role of S in enhancing the catalytic performance of Fe/C-based catalysts for PMS activation, which would provide meaningful insights into the design of high-performance PMS activators for the sustainable remediation of emerging contaminants-polluted water bodies.
过一硫酸盐（PMS）介导的高级氧化过程因其高处理能力和相对低成本，在降解废水中的抗生素（如四环素（TC））方面越来越受到关注，然而设计高效的PMS活化催化剂仍然是一个挑战。在本研究中，开发了一种由铁基金属有机框架（Fe-MOFs）合成的硫掺杂Fe/C催化剂（Fe@C-S）用于活化PMS以去除TC。在最佳条件下，Fe@C-S150/PMS体系在40分钟内对TC的去除效率为91.2%。同时，Fe@C-S150/PMS体系的k值（0.2038 min⁻¹）是不含硫的Fe@C基PMS体系的3.36倍。此外，Fe@C-S150/PMS体系在不同水基质中表现出高稳定性。进一步研究发现，TC的降解机制主要归因于非自由基途径（单线态氧和电子转移）。催化剂上的铁纳米颗粒、硫和羰基均参与了活性氧物种（ROS）的生成。此外，硫物种可以增强Fe²⁺/Fe³⁺的氧化还原循环并加速电子转移过程。这项工作突出了硫在增强Fe/C基催化剂活化PMS的催化性能方面的关键作用，这将为设计用于可持续修复新兴污染物污染水体的高性能PMS活化剂提供有意义的见解。
