{"title":"解密可持续芬顿氧化作用的新型烟酸锰(II)/过氧单硫酸盐体系:烟酸锰(IV)过氧化单硫酸盐复合物的优势","authors":"Lijun Niu, Zhipeng Luo, Wenzheng Chen, Xinyang Zhong, Huabin Zeng, Xin Yu, Mingbao Feng","doi":"10.1021/acs.est.4c05482","DOIUrl":null,"url":null,"abstract":"A highly efficient and sustainable water treatment system was developed herein by combining Mn(II), peroxymonosulfate (PMS), and biodegradable picolinic acid (PICA). The micropollutant elimination process underwent two phases: an initial slow degradation phase (0–10 min) followed by a rapid phase (10–20 min). Multiple evidence demonstrated that a PICA-Mn(IV) complex (PICA-Mn(IV)*) was generated, acting as a conductive bridge facilitating the electron transfer between PMS and micropollutants. Quantum chemical calculations revealed that PMS readily oxidized the PICA-Mn(II)* to PICA-Mn(IV)*. This intermediate then complexed with PMS to produce PICA-Mn(IV)-PMS*, elongating the O–O bond of PMS and increasing its oxidation capacity. The primary transformation mechanisms of typical micropollutants mediated by PICA-Mn(IV)-PMS* include oxidation, ring-opening, bond cleavage, and epoxidation reactions. The toxicity assessment results showed that most products were less toxic than the parent compounds. Moreover, the Mn(II)/PICA/PMS system showed resilience to water matrices and high efficiency in real water environments. Notably, PICA-Mn(IV)* exhibited greater stability and a longer lifespan than traditional reactive oxygen species, enabling repeated utilization. Overall, this study developed an innovative, sustainable, and selective oxidation system, i.e., Mn(II)/PICA/PMS, for rapid water decontamination, highlighting the critical role of in situ generated Mn(IV).","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8000,"publicationDate":"2024-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Deciphering the Novel Picolinate-Mn(II)/peroxymonosulfate System for Sustainable Fenton-like Oxidation: Dominance of the Picolinate-Mn(IV)-peroxymonosulfate Complex\",\"authors\":\"Lijun Niu, Zhipeng Luo, Wenzheng Chen, Xinyang Zhong, Huabin Zeng, Xin Yu, Mingbao Feng\",\"doi\":\"10.1021/acs.est.4c05482\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"A highly efficient and sustainable water treatment system was developed herein by combining Mn(II), peroxymonosulfate (PMS), and biodegradable picolinic acid (PICA). The micropollutant elimination process underwent two phases: an initial slow degradation phase (0–10 min) followed by a rapid phase (10–20 min). Multiple evidence demonstrated that a PICA-Mn(IV) complex (PICA-Mn(IV)*) was generated, acting as a conductive bridge facilitating the electron transfer between PMS and micropollutants. Quantum chemical calculations revealed that PMS readily oxidized the PICA-Mn(II)* to PICA-Mn(IV)*. This intermediate then complexed with PMS to produce PICA-Mn(IV)-PMS*, elongating the O–O bond of PMS and increasing its oxidation capacity. The primary transformation mechanisms of typical micropollutants mediated by PICA-Mn(IV)-PMS* include oxidation, ring-opening, bond cleavage, and epoxidation reactions. The toxicity assessment results showed that most products were less toxic than the parent compounds. Moreover, the Mn(II)/PICA/PMS system showed resilience to water matrices and high efficiency in real water environments. Notably, PICA-Mn(IV)* exhibited greater stability and a longer lifespan than traditional reactive oxygen species, enabling repeated utilization. Overall, this study developed an innovative, sustainable, and selective oxidation system, i.e., Mn(II)/PICA/PMS, for rapid water decontamination, highlighting the critical role of in situ generated Mn(IV).\",\"PeriodicalId\":36,\"journal\":{\"name\":\"环境科学与技术\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":10.8000,\"publicationDate\":\"2024-09-14\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"环境科学与技术\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.est.4c05482\",\"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":"环境科学与技术","FirstCategoryId":"1","ListUrlMain":"https://doi.org/10.1021/acs.est.4c05482","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}
Deciphering the Novel Picolinate-Mn(II)/peroxymonosulfate System for Sustainable Fenton-like Oxidation: Dominance of the Picolinate-Mn(IV)-peroxymonosulfate Complex
A highly efficient and sustainable water treatment system was developed herein by combining Mn(II), peroxymonosulfate (PMS), and biodegradable picolinic acid (PICA). The micropollutant elimination process underwent two phases: an initial slow degradation phase (0–10 min) followed by a rapid phase (10–20 min). Multiple evidence demonstrated that a PICA-Mn(IV) complex (PICA-Mn(IV)*) was generated, acting as a conductive bridge facilitating the electron transfer between PMS and micropollutants. Quantum chemical calculations revealed that PMS readily oxidized the PICA-Mn(II)* to PICA-Mn(IV)*. This intermediate then complexed with PMS to produce PICA-Mn(IV)-PMS*, elongating the O–O bond of PMS and increasing its oxidation capacity. The primary transformation mechanisms of typical micropollutants mediated by PICA-Mn(IV)-PMS* include oxidation, ring-opening, bond cleavage, and epoxidation reactions. The toxicity assessment results showed that most products were less toxic than the parent compounds. Moreover, the Mn(II)/PICA/PMS system showed resilience to water matrices and high efficiency in real water environments. Notably, PICA-Mn(IV)* exhibited greater stability and a longer lifespan than traditional reactive oxygen species, enabling repeated utilization. Overall, this study developed an innovative, sustainable, and selective oxidation system, i.e., Mn(II)/PICA/PMS, for rapid water decontamination, highlighting the critical role of in situ generated Mn(IV).
期刊介绍:
Environmental Science & Technology (ES&T) is a co-sponsored academic and technical magazine by the Hubei Provincial Environmental Protection Bureau and the Hubei Provincial Academy of Environmental Sciences.
Environmental Science & Technology (ES&T) holds the status of Chinese core journals, scientific papers source journals of China, Chinese Science Citation Database source journals, and Chinese Academic Journal Comprehensive Evaluation Database source journals. This publication focuses on the academic field of environmental protection, featuring articles related to environmental protection and technical advancements.