The regulation of generation rate facilitates the win–win of ROS yield and utilization efficiency in heterogeneous persulfate catalytic oxidation system

• Published in: Separation and purification technology 2023-10, Vol.323, p.124389, Article 124389
• Main Authors: Zhou, Xinquan, Zhang, Luyun, Wang, Hui, Lu, Weiwei, Zhang, Ruichang, Li, Hanxiang, Li, Jun, Wei, Xuefeng
• Format: Article
• Language: English
• Subjects: AOPs; Phosphate; PMS; Reactive oxygen species; Utilization efficiency
• ISSN: 1383-5866; 1873-3794
• DOI: 10.1016/j.seppur.2023.124389

[Display omitted] •The introduction of MgO (CaO) enhanced PMS activation efficiency of CuOMgO (CuOCaO);•OVs on CuOMgO (CuOCaO) induced PMS rapid decomposition/ROS rapid generation;•The rapid production of ROS reduced its utilization efficiency;•The utilization efficiency of 1O2 was increased by adjusting the contact frequency between catalyst and PMS. Heterogeneous catalytic oxidation is one of the most effective methods to degrade various and complex organic pollutants in aqueous solution. Increasing reactive oxygen species (ROS) yield has always been the main objective to improve the oxidation efficiency. However, the mass production of ROS in a short time is inevitably faced with self-quenching and ineffective consumption. Herein, Cu-based composite oxides (CuOMOx) (M = Ca, Mg, Zn, Mn) were synthesized and used for catalytic activation of permonosulfate (PMS). Although the introduction of unreducible metal oxides significantly improved the activation efficiency of PMS, the abnormal phenomenon of lower substrate degradation efficiency and PMS stoichiometry appeared. The underlying mechanism is that the rapid production of ROS results in a mismatch of the production/effective consumption ratio, which causes massive ROS disappeared naturally before attacking the substrate. In this scenario, reasonable regulation of ROS generation rate by phosphate addition improved the utilization efficiency of ROS without affecting its yield. Our finding is beneficial to achieve a win–win situation of ROS yield and utilization efficiency in heterogeneous catalytic oxidation systems.