Xiaoyue Duan , Ziqi Ning , Xinyu Sui , Shiyu Geng , Hailong Wang , Chunbo Liu , Limin Chang
{"title":"超声辅助电催化降解微塑料的疏水性Ce3Mn7-PbO2阳极:增强的性能和降解机制","authors":"Xiaoyue Duan , Ziqi Ning , Xinyu Sui , Shiyu Geng , Hailong Wang , Chunbo Liu , Limin Chang","doi":"10.1016/j.jece.2025.116207","DOIUrl":null,"url":null,"abstract":"<div><div>Microplastics (MPs), as emerging organic pollutants, pose significant threats to water environment safety and human health. In this study, a highly hydrophobic Ce<sub>3</sub>Mn<sub>7</sub>-PbO<sub>2</sub> (HH-Ce<sub>3</sub>Mn<sub>7</sub>-PbO<sub>2</sub>) anode was developed and applied in ultrasound-assisted electrochemical oxidation (UEO) system for the degradation of MPs. The incorporation of Ce<sub>3</sub>Mn<sub>7</sub> and enhanced hydrophobicity improved the stability of the PbO<sub>2</sub> anode and facilitated the generation of hydroxyl radicals (•OH). The introduction of ultrasound led to the formation of hot spots, which not only enhanced chemical reaction and mass transfer but also increased the production of reactive oxygen species (ROS). Consequently, during the degradation of polyvinyl chloride microplastics (PVC-MPs), the UEO system with the HH-Ce<sub>3</sub>Mn<sub>7</sub>-PbO<sub>2</sub> anode achieved significantly higher degradation efficiency of 71.5 %, compared to 24.7 % observed in conventional electrochemical oxidation (EO) system using a pure PbO<sub>2</sub> anode. Electron spin resonance (ESR) tests and reactive species quenching experiments revealed that the •OH was the primary reactive species, contributing 67.4 % to the degradation process. In contrast, the contributions of sulfate radical (SO<sub>4</sub><sup>•−</sup>), superoxide radical (O<sub>2</sub><sup>•−</sup>), and singlet oxygen (<sup>1</sup>O<sub>2</sub>) were relatively minor, at 7.3 %, 15.3 %, and 10.0 %, respectively. These findings provide a scientific foundation and theoretical insights for the efficient degradation of MPs through the UEO process.</div></div>","PeriodicalId":15759,"journal":{"name":"Journal of Environmental Chemical Engineering","volume":"13 3","pages":"Article 116207"},"PeriodicalIF":7.4000,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Ultrasound-assisted electrocatalytic degradation of microplastics by a hydrophobic Ce3Mn7-PbO2 anode: Enhanced performance and degradation mechanism\",\"authors\":\"Xiaoyue Duan , Ziqi Ning , Xinyu Sui , Shiyu Geng , Hailong Wang , Chunbo Liu , Limin Chang\",\"doi\":\"10.1016/j.jece.2025.116207\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Microplastics (MPs), as emerging organic pollutants, pose significant threats to water environment safety and human health. In this study, a highly hydrophobic Ce<sub>3</sub>Mn<sub>7</sub>-PbO<sub>2</sub> (HH-Ce<sub>3</sub>Mn<sub>7</sub>-PbO<sub>2</sub>) anode was developed and applied in ultrasound-assisted electrochemical oxidation (UEO) system for the degradation of MPs. The incorporation of Ce<sub>3</sub>Mn<sub>7</sub> and enhanced hydrophobicity improved the stability of the PbO<sub>2</sub> anode and facilitated the generation of hydroxyl radicals (•OH). The introduction of ultrasound led to the formation of hot spots, which not only enhanced chemical reaction and mass transfer but also increased the production of reactive oxygen species (ROS). Consequently, during the degradation of polyvinyl chloride microplastics (PVC-MPs), the UEO system with the HH-Ce<sub>3</sub>Mn<sub>7</sub>-PbO<sub>2</sub> anode achieved significantly higher degradation efficiency of 71.5 %, compared to 24.7 % observed in conventional electrochemical oxidation (EO) system using a pure PbO<sub>2</sub> anode. Electron spin resonance (ESR) tests and reactive species quenching experiments revealed that the •OH was the primary reactive species, contributing 67.4 % to the degradation process. In contrast, the contributions of sulfate radical (SO<sub>4</sub><sup>•−</sup>), superoxide radical (O<sub>2</sub><sup>•−</sup>), and singlet oxygen (<sup>1</sup>O<sub>2</sub>) were relatively minor, at 7.3 %, 15.3 %, and 10.0 %, respectively. These findings provide a scientific foundation and theoretical insights for the efficient degradation of MPs through the UEO process.</div></div>\",\"PeriodicalId\":15759,\"journal\":{\"name\":\"Journal of Environmental Chemical Engineering\",\"volume\":\"13 3\",\"pages\":\"Article 116207\"},\"PeriodicalIF\":7.4000,\"publicationDate\":\"2025-03-17\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Environmental Chemical Engineering\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2213343725009030\",\"RegionNum\":2,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Environmental Chemical Engineering","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2213343725009030","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Ultrasound-assisted electrocatalytic degradation of microplastics by a hydrophobic Ce3Mn7-PbO2 anode: Enhanced performance and degradation mechanism
Microplastics (MPs), as emerging organic pollutants, pose significant threats to water environment safety and human health. In this study, a highly hydrophobic Ce3Mn7-PbO2 (HH-Ce3Mn7-PbO2) anode was developed and applied in ultrasound-assisted electrochemical oxidation (UEO) system for the degradation of MPs. The incorporation of Ce3Mn7 and enhanced hydrophobicity improved the stability of the PbO2 anode and facilitated the generation of hydroxyl radicals (•OH). The introduction of ultrasound led to the formation of hot spots, which not only enhanced chemical reaction and mass transfer but also increased the production of reactive oxygen species (ROS). Consequently, during the degradation of polyvinyl chloride microplastics (PVC-MPs), the UEO system with the HH-Ce3Mn7-PbO2 anode achieved significantly higher degradation efficiency of 71.5 %, compared to 24.7 % observed in conventional electrochemical oxidation (EO) system using a pure PbO2 anode. Electron spin resonance (ESR) tests and reactive species quenching experiments revealed that the •OH was the primary reactive species, contributing 67.4 % to the degradation process. In contrast, the contributions of sulfate radical (SO4•−), superoxide radical (O2•−), and singlet oxygen (1O2) were relatively minor, at 7.3 %, 15.3 %, and 10.0 %, respectively. These findings provide a scientific foundation and theoretical insights for the efficient degradation of MPs through the UEO process.
期刊介绍:
The Journal of Environmental Chemical Engineering (JECE) serves as a platform for the dissemination of original and innovative research focusing on the advancement of environmentally-friendly, sustainable technologies. JECE emphasizes the transition towards a carbon-neutral circular economy and a self-sufficient bio-based economy. Topics covered include soil, water, wastewater, and air decontamination; pollution monitoring, prevention, and control; advanced analytics, sensors, impact and risk assessment methodologies in environmental chemical engineering; resource recovery (water, nutrients, materials, energy); industrial ecology; valorization of waste streams; waste management (including e-waste); climate-water-energy-food nexus; novel materials for environmental, chemical, and energy applications; sustainability and environmental safety; water digitalization, water data science, and machine learning; process integration and intensification; recent developments in green chemistry for synthesis, catalysis, and energy; and original research on contaminants of emerging concern, persistent chemicals, and priority substances, including microplastics, nanoplastics, nanomaterials, micropollutants, antimicrobial resistance genes, and emerging pathogens (viruses, bacteria, parasites) of environmental significance.