Xiang Chen , Tao Guo , Tiezhu Yan , Yunrong Dai , Lifeng Yin
{"title":"电场调节下选择性生成羟基和硫酸根自由基以降解微污染物:机理与结构-活性关系","authors":"Xiang Chen , Tao Guo , Tiezhu Yan , Yunrong Dai , Lifeng Yin","doi":"10.1016/j.jhazmat.2024.136513","DOIUrl":null,"url":null,"abstract":"<div><div>Peroxymonosulfate (PMS) activation generates potent reactive oxygen species (ROS) such as sulfate radical (SO<sub>4</sub><sup>·–</sup>) and hydroxyl radical (·OH), which play a key role in organic pollutant degradation. However, controlling the generation of these free radicals remains challenging. In this study, various metal (Co, Ni, and Cu)-doped nitrogen carbon compounds (NCs) were synthesized, and their performance in PMS activation under electric field regulation was explored to modulate ROS production for selective pollutant degradation. Bisphenol A (BPA), a readily degradable compound, and ibuprofen (IBU), a recalcitrant pollutant, were chosen as model pollutants to assess degradation efficiency. All catalysts achieved over 95 % BPA removal without the electric field, but the application of an electric field significantly accelerated BPA degradation, achieving complete removal within 3 min. In contrast, IBU degradation showed significant variation depending on the catalyst used and the electric field intensity, with Cu-NC demonstrating the highest performance, enhancing the degradation rate by 3.78-fold. Mechanistic studies revealed that the electric field altered the electron density on the catalyst surface, shifting ROS production from SO<sub>4</sub><sup>·–</sup> to·OH in Co-NC systems. The findings could provide valuable insights into PMS activation under electric field regulation, offering a novel strategy for enhancing micropollutant removal through controlled ROS generation.</div></div>","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"481 ","pages":"Article 136513"},"PeriodicalIF":12.2000,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Selective generation of hydroxyl and sulfate radicals under electric field regulation for micropollutants degradation: Mechanism and structure-activity relationship\",\"authors\":\"Xiang Chen , Tao Guo , Tiezhu Yan , Yunrong Dai , Lifeng Yin\",\"doi\":\"10.1016/j.jhazmat.2024.136513\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Peroxymonosulfate (PMS) activation generates potent reactive oxygen species (ROS) such as sulfate radical (SO<sub>4</sub><sup>·–</sup>) and hydroxyl radical (·OH), which play a key role in organic pollutant degradation. However, controlling the generation of these free radicals remains challenging. In this study, various metal (Co, Ni, and Cu)-doped nitrogen carbon compounds (NCs) were synthesized, and their performance in PMS activation under electric field regulation was explored to modulate ROS production for selective pollutant degradation. Bisphenol A (BPA), a readily degradable compound, and ibuprofen (IBU), a recalcitrant pollutant, were chosen as model pollutants to assess degradation efficiency. All catalysts achieved over 95 % BPA removal without the electric field, but the application of an electric field significantly accelerated BPA degradation, achieving complete removal within 3 min. In contrast, IBU degradation showed significant variation depending on the catalyst used and the electric field intensity, with Cu-NC demonstrating the highest performance, enhancing the degradation rate by 3.78-fold. Mechanistic studies revealed that the electric field altered the electron density on the catalyst surface, shifting ROS production from SO<sub>4</sub><sup>·–</sup> to·OH in Co-NC systems. The findings could provide valuable insights into PMS activation under electric field regulation, offering a novel strategy for enhancing micropollutant removal through controlled ROS generation.</div></div>\",\"PeriodicalId\":361,\"journal\":{\"name\":\"Journal of Hazardous Materials\",\"volume\":\"481 \",\"pages\":\"Article 136513\"},\"PeriodicalIF\":12.2000,\"publicationDate\":\"2024-11-16\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Hazardous Materials\",\"FirstCategoryId\":\"93\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0304389424030929\",\"RegionNum\":1,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, ENVIRONMENTAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Hazardous Materials","FirstCategoryId":"93","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0304389424030929","RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}
Selective generation of hydroxyl and sulfate radicals under electric field regulation for micropollutants degradation: Mechanism and structure-activity relationship
Peroxymonosulfate (PMS) activation generates potent reactive oxygen species (ROS) such as sulfate radical (SO4·–) and hydroxyl radical (·OH), which play a key role in organic pollutant degradation. However, controlling the generation of these free radicals remains challenging. In this study, various metal (Co, Ni, and Cu)-doped nitrogen carbon compounds (NCs) were synthesized, and their performance in PMS activation under electric field regulation was explored to modulate ROS production for selective pollutant degradation. Bisphenol A (BPA), a readily degradable compound, and ibuprofen (IBU), a recalcitrant pollutant, were chosen as model pollutants to assess degradation efficiency. All catalysts achieved over 95 % BPA removal without the electric field, but the application of an electric field significantly accelerated BPA degradation, achieving complete removal within 3 min. In contrast, IBU degradation showed significant variation depending on the catalyst used and the electric field intensity, with Cu-NC demonstrating the highest performance, enhancing the degradation rate by 3.78-fold. Mechanistic studies revealed that the electric field altered the electron density on the catalyst surface, shifting ROS production from SO4·– to·OH in Co-NC systems. The findings could provide valuable insights into PMS activation under electric field regulation, offering a novel strategy for enhancing micropollutant removal through controlled ROS generation.
期刊介绍:
The Journal of Hazardous Materials serves as a global platform for promoting cutting-edge research in the field of Environmental Science and Engineering. Our publication features a wide range of articles, including full-length research papers, review articles, and perspectives, with the aim of enhancing our understanding of the dangers and risks associated with various materials concerning public health and the environment. It is important to note that the term "environmental contaminants" refers specifically to substances that pose hazardous effects through contamination, while excluding those that do not have such impacts on the environment or human health. Moreover, we emphasize the distinction between wastes and hazardous materials in order to provide further clarity on the scope of the journal. We have a keen interest in exploring specific compounds and microbial agents that have adverse effects on the environment.