Liu Xinyue, Yan Xinyi, Liu Wenyuan, Yan Qingyun, Xing Mingyang
Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Frontiers Science Center for Materiobiology and Dynamic Chemistry, Institute of Fine Chemicals, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, China.
Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Frontiers Science Center for Materiobiology and Dynamic Chemistry, Institute of Fine Chemicals, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, China; Shanghai Engineering Research Center for Multi-media Environmental Catalysis and Resource Utilization, East China University of Science and Technology, Shanghai 200237, China.
Sci Bull (Beijing). 2023 Mar 30;68(6):603-612. doi: 10.1016/j.scib.2023.02.031. Epub 2023 Feb 24.
Coexistence of radical and nonradical reaction pathways during advanced oxidation processes (AOPs) makes it challenging to obtain flexible regulation of high efficiency and selectivity for the requirement of diverse degradation. Herein, a series of FeO/MoOS samples coupling peroxymonosulfate (PMS) systems enabled the switching of radical and nonradical pathways through the inclusion of defects and adjustment of Mo/Mo ratios. The silicon cladding operation introduced defects by disrupting the original lattice of FeO and MoOS. Meanwhile, the abundance of defective electrons increased the amount of Mo on the catalyst surface, promoting PMS decomposition with a maximum k value up to 1.530 min and a maximum free radical contribution of 81.33%. The Mo/Mo ratio in the catalyst was similarly altered by different Fe contents, and Mo contributed to the production of O, allowing the whole system to attain a nonradical species-dominated (68.26%) pathway. The radical species-dominated system has a high chemical oxygen demand (COD) removal rate for actual wastewater treatment. Conversely, the nonradical species-dominated system can considerably improve the biodegradability of wastewater (biochemical oxygen demand (BOD)/COD = 0.997). The tunable hybrid reaction pathways will expand the targeted applications of AOPs.
在高级氧化过程(AOPs)中,自由基和非自由基反应途径共存,这使得针对不同降解需求实现高效性和选择性的灵活调控具有挑战性。在此,一系列FeO/MoOS样品与过一硫酸盐(PMS)体系相结合,通过引入缺陷和调整Mo/Mo比例实现了自由基和非自由基途径的切换。硅包覆操作通过破坏FeO和MoOS的原始晶格引入了缺陷。同时,大量缺陷电子增加了催化剂表面的Mo含量,促进了PMS的分解,最大k值高达1.530 min,自由基贡献最大值为81.33%。催化剂中的Mo/Mo比例也因不同的Fe含量而发生类似变化,Mo有助于O的产生,使整个体系实现以非自由基物种为主导(68.26%)的途径。以自由基物种为主导的体系在实际废水处理中具有较高的化学需氧量(COD)去除率。相反,以非自由基物种为主导的体系可显著提高废水的生物降解性(生化需氧量(BOD)/COD = 0.997)。可调控的混合反应途径将拓展AOPs的靶向应用。