Jin Limin, You Shijie, Ren Nanqi, Liu Yanbiao
College of Environmental Science and Engineering, Textile Pollution Controlling Engineering Center of the Ministry of Ecology and Environment, Donghua University, 2999 North Renmin Road, Shanghai 201620, China.
State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China.
Fundam Res. 2022 Mar 18;3(5):770-776. doi: 10.1016/j.fmre.2022.03.005. eCollection 2023 Sep.
Defect engineering is an effective strategy to boost the catalytic activity of MXene towards heterogeneous peroxymonosulfate (PMS) activation for water decontamination. Herein, we developed a facile approach to fine-tune the generation of oxygen vacancies (OVs) on TiCNT crystals by Ce-doping (Ce-TiCNT) with the aim of mediating PMS activation for the degradation of micropollutants in water. By varying the dopant content, the OV concentrations of TiCNT could be varied to enable the activation of PMS to almost 100% singlet oxygen (O), and hence the effective degradation of sulfamethoxazole (SMX, a model micropollutant). Various advanced characterization techniques were employed to obtain detailed information on the microstructure, morphology, and defect states of the catalysts. The experimental results showed that SMX removal was proportional to the OVs level. Density functional theory (DFT) models demonstrated that, in contrast to pristine TiCNT, the OVs on 10%Ce-TiCNT could adsorb the terminal O of PMS, which facilitated the formation of SO as well as the generation of O. We further loaded the optimized catalysts onto a polytetrafluoroethylene microfiltration membrane and also demonstrated the efficient removal of SMX from water using a convection-enhanced mass transport flow-through configuration. This study provides new insights into the effective removal of micropollutants from water by integrating state-of-the-art defect engineering, advanced oxidation, and microfiltration techniques.
缺陷工程是提高MXene对非均相过一硫酸盐（PMS）活化以进行水净化的催化活性的有效策略。在此，我们开发了一种简便的方法，通过Ce掺杂（Ce-TiCNT）来微调TiCNT晶体上氧空位（OVs）的生成，目的是介导PMS活化以降解水中的微污染物。通过改变掺杂剂含量，可以改变TiCNT的OV浓度，使PMS活化生成近100%的单线态氧（O），从而有效降解磺胺甲恶唑（SMX，一种典型的微污染物）。采用了各种先进的表征技术来获取有关催化剂微观结构、形态和缺陷状态的详细信息。实验结果表明，SMX的去除与OVs水平成正比。密度泛函理论（DFT）模型表明，与原始TiCNT相比，10%Ce-TiCNT上的OVs可以吸附PMS的末端O，这促进了SO的形成以及O的生成。我们进一步将优化后的催化剂负载到聚四氟乙烯微滤膜上，并通过对流增强传质流通配置证明了从水中有效去除SMX。本研究通过整合先进的缺陷工程、高级氧化和微滤技术，为从水中有效去除微污染物提供了新的见解。
