Advanced oxidation processes (AOPs) based on peroxymonosulfate (PMS) enable efficient generation of highly oxidative radicals for eliminating diverse organic pollutants. Developing multi-active, stable catalysts remains challenging. In this study, a composite catalyst integrating high-entropy perovskite oxides (HEPs) with carbon microspheres (CS), denoted as HEPs@CS, was successfully synthesized to activate PMS for generating reactive oxygen species (ROS), enabling efficient degradation of Rhodamine B (RhB, 99.7 % removal in 10 min), tetracycline (TC), and other pollutants via a singlet oxygen (1O2)-dominated nonradical pathway, with a high rate constant (0.5815 min-1). The HEPs framework, featuring a multi-active-site co-catalytic system and strong metal-support interactions (MSI), exhibited exceptional catalytic activity and stability. Through EPR, FT-IR, and Raman characterization tests, the material's exceptional performance is also attributed to the synergistic participation of oxygen vacancies (OV), diverse carbon surface functional groups, and defect structures in the reaction system. These factors collectively enhance electron transfer during both PMS activation and pollutant degradation processes. ECOSAR software confirmed the environmental safety of this process. Our findings demonstrate that HEPs@CS exhibits outstanding performance as a PMS activator for wastewater treatment of organic pollutants. This work provides deeper insights into how polymetallic electronic structures in high-entropy perovskites modulate PMS activation mechanisms.

中文翻译：

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高熵钙钛矿嵌入碳基催化剂中，用于过氧一硫酸盐活化以降解罗丹明 B：性能和机理见解

基于过氧一硫酸盐 （PMS） 的高级氧化过程 （AOP） 能够有效产生高氧化自由基，以消除各种有机污染物。开发多活性、稳定的催化剂仍然具有挑战性。在本研究中，成功合成了一种将高熵钙钛矿氧化物 （HEP） 与碳微球 （CS） 集成的复合催化剂，以 HEPs@CS 表示，以激活 PMS 以产生活性氧 （ROS），从而能够通过单线态氧 （1O2） 为主的非自由基途径高效降解罗丹明 B （RhB，10 分钟内去除 99.7%）、四环素 （TC） 和其他污染物，具有高速率常数 （0.5815 min-1）。HEPs 框架具有多活性位点共催化系统和强金属-支持相互作用 （MSI），表现出卓越的催化活性和稳定性。通过 EPR、FT-IR 和拉曼表征测试，该材料的卓越性能还归因于反应体系中氧空位 （OV）、不同碳表面官能团和缺陷结构的协同参与。这些因素共同增强了 PMS 活化和污染物降解过程中的电子转移。ECOSAR 软件证实了该工艺的环境安全性。我们的研究结果表明，HEPs@CS 作为有机污染物废水处理的 PMS 活化剂表现出出色的性能。这项工作为高熵钙钛矿中的多金属电子结构如何调节 PMS 激活机制提供了更深入的见解。