Zhi Gao, Yu-Lei Liu, Zhuang-Song Huang, Xiao-Na Zhao, Xian-Shi Wang, Zi-Yi Han, Chong-Wei Cui, Jun Ma, Lu Wang
{"title":"为高效氧化定制铁(VI)配位微环境:配体驱动的电子转移和聚合转向","authors":"Zhi Gao, Yu-Lei Liu, Zhuang-Song Huang, Xiao-Na Zhao, Xian-Shi Wang, Zi-Yi Han, Chong-Wei Cui, Jun Ma, Lu Wang","doi":"10.1038/s41545-025-00488-w","DOIUrl":null,"url":null,"abstract":"<p>Utilizing ligand-mediated homogeneous catalysis to enhance oxidant-driven pollutant removal efficiency presents significant research value while posing substantial challenges. This study utilized ethylenediaminetetraacetic acid (EDTA) to alter the coordination environment of ferrate(VI), thereby steering electron transfer and the phenoxylation pathways to enhance the pollutant removal, which is realized by the complexation-mediated regulation for kinetics and thermodynamics. For example, the introduction of EDTA increased the rate constant of ferrate(VI) oxidizing phenol by four times (from 50.79 M<sup>−1</sup> s<sup>−1</sup> to 208 M<sup>−1</sup> s<sup>−1</sup>) and the stoichiometric ratio (∆[phenol]/∆[K<sub>2</sub>FeO<sub>4</sub>]) from 0.17:1 to 0.22:1. Theoretical calculation and experimental characterization proved that the in-situ formed metastable Fe(VI)-EDTA complex facilitates the electron transfer from Fe(VI) to benzene ring and the phenoxylation pathways. Consequently, the related polymerization products were produced in greater quantities (about 5 times) and with broader diversity than Fe(VI) alone. In the application to real water, the introduction of EDTA reduced more than half of ferrate(VI)’s dosage previously required for completely removing phenol. This study presents a novel strategy for optimizing ferrate(VI) oxidizing pollutants in water treatment, which presents notable environmental benefits by minimizing ferrate(VI) consumption and enhancing pollutant removal efficiency.</p><figure></figure>","PeriodicalId":19375,"journal":{"name":"npj Clean Water","volume":"36 1","pages":""},"PeriodicalIF":10.4000,"publicationDate":"2025-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Tailoring Fe(VI) coordination microenvironment for high-efficiency oxidation: ligand-driven electron transfer and polymerization steering\",\"authors\":\"Zhi Gao, Yu-Lei Liu, Zhuang-Song Huang, Xiao-Na Zhao, Xian-Shi Wang, Zi-Yi Han, Chong-Wei Cui, Jun Ma, Lu Wang\",\"doi\":\"10.1038/s41545-025-00488-w\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Utilizing ligand-mediated homogeneous catalysis to enhance oxidant-driven pollutant removal efficiency presents significant research value while posing substantial challenges. This study utilized ethylenediaminetetraacetic acid (EDTA) to alter the coordination environment of ferrate(VI), thereby steering electron transfer and the phenoxylation pathways to enhance the pollutant removal, which is realized by the complexation-mediated regulation for kinetics and thermodynamics. For example, the introduction of EDTA increased the rate constant of ferrate(VI) oxidizing phenol by four times (from 50.79 M<sup>−1</sup> s<sup>−1</sup> to 208 M<sup>−1</sup> s<sup>−1</sup>) and the stoichiometric ratio (∆[phenol]/∆[K<sub>2</sub>FeO<sub>4</sub>]) from 0.17:1 to 0.22:1. Theoretical calculation and experimental characterization proved that the in-situ formed metastable Fe(VI)-EDTA complex facilitates the electron transfer from Fe(VI) to benzene ring and the phenoxylation pathways. Consequently, the related polymerization products were produced in greater quantities (about 5 times) and with broader diversity than Fe(VI) alone. In the application to real water, the introduction of EDTA reduced more than half of ferrate(VI)’s dosage previously required for completely removing phenol. This study presents a novel strategy for optimizing ferrate(VI) oxidizing pollutants in water treatment, which presents notable environmental benefits by minimizing ferrate(VI) consumption and enhancing pollutant removal efficiency.</p><figure></figure>\",\"PeriodicalId\":19375,\"journal\":{\"name\":\"npj Clean Water\",\"volume\":\"36 1\",\"pages\":\"\"},\"PeriodicalIF\":10.4000,\"publicationDate\":\"2025-07-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"npj Clean Water\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://doi.org/10.1038/s41545-025-00488-w\",\"RegionNum\":1,\"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":"npj Clean Water","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1038/s41545-025-00488-w","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Tailoring Fe(VI) coordination microenvironment for high-efficiency oxidation: ligand-driven electron transfer and polymerization steering
Utilizing ligand-mediated homogeneous catalysis to enhance oxidant-driven pollutant removal efficiency presents significant research value while posing substantial challenges. This study utilized ethylenediaminetetraacetic acid (EDTA) to alter the coordination environment of ferrate(VI), thereby steering electron transfer and the phenoxylation pathways to enhance the pollutant removal, which is realized by the complexation-mediated regulation for kinetics and thermodynamics. For example, the introduction of EDTA increased the rate constant of ferrate(VI) oxidizing phenol by four times (from 50.79 M−1 s−1 to 208 M−1 s−1) and the stoichiometric ratio (∆[phenol]/∆[K2FeO4]) from 0.17:1 to 0.22:1. Theoretical calculation and experimental characterization proved that the in-situ formed metastable Fe(VI)-EDTA complex facilitates the electron transfer from Fe(VI) to benzene ring and the phenoxylation pathways. Consequently, the related polymerization products were produced in greater quantities (about 5 times) and with broader diversity than Fe(VI) alone. In the application to real water, the introduction of EDTA reduced more than half of ferrate(VI)’s dosage previously required for completely removing phenol. This study presents a novel strategy for optimizing ferrate(VI) oxidizing pollutants in water treatment, which presents notable environmental benefits by minimizing ferrate(VI) consumption and enhancing pollutant removal efficiency.
npj Clean WaterEnvironmental Science-Water Science and Technology
CiteScore
15.30
自引率
2.60%
发文量
61
审稿时长
5 weeks
期刊介绍:
npj Clean Water publishes high-quality papers that report cutting-edge science, technology, applications, policies, and societal issues contributing to a more sustainable supply of clean water. The journal's publications may also support and accelerate the achievement of Sustainable Development Goal 6, which focuses on clean water and sanitation.