Zhenyi Chen, Shuo Li, Kun Feng, Zhen Wen and Jun Zhong
{"title":"接触电催化中中心原子氧化促进Co(II)-EDTA解复","authors":"Zhenyi Chen, Shuo Li, Kun Feng, Zhen Wen and Jun Zhong","doi":"10.1039/D5CP01566A","DOIUrl":null,"url":null,"abstract":"<p >Low-level radioactive wastewater containing Co(<small>II</small>)–EDTA generated in the nuclear industry is harmful to the environment, but it is difficult to remove owing to the high stability of metal–organic complexes. Here, we report efficient contact-electro-catalysis (CEC) to achieve the decomplexation of Co(<small>II</small>)–EDTA by using commercial fluorinated ethylene propylene (FEP) powder as a dielectric catalyst. The reaction generated reactive oxygen species through solid–liquid interfacial charge transfer, disrupting the chemical bonds and then oxidizing the central atoms in Co(<small>II</small>)–EDTA to form Co(<small>III</small>)–EDTA with vacancies. The Co(<small>III</small>)–EDTA could be easily removed from the solution under alkaline conditions. The decomplexation efficiency reached a high value of 41.6%, with a constant reaction rate of 0.024 min<small><sup>−1</sup></small> in 240 minutes. The FEP also exhibited excellent recyclability over 40 h without obvious changes. Unlike conventional advanced oxidation processes, this approach does not require the use of electrodes or chemical oxidants, leading to low energy consumption. This approach also holds great potential for green wastewater management <em>via</em> integration with ambient mechanical energy sources (<em>e.g.</em>, wind and hydrostatic pressure).</p>","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":" 29","pages":" 15742-15748"},"PeriodicalIF":2.9000,"publicationDate":"2025-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Promoting Co(ii)–EDTA decomplexation by central atom oxidation in contact-electro-catalysis†\",\"authors\":\"Zhenyi Chen, Shuo Li, Kun Feng, Zhen Wen and Jun Zhong\",\"doi\":\"10.1039/D5CP01566A\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Low-level radioactive wastewater containing Co(<small>II</small>)–EDTA generated in the nuclear industry is harmful to the environment, but it is difficult to remove owing to the high stability of metal–organic complexes. Here, we report efficient contact-electro-catalysis (CEC) to achieve the decomplexation of Co(<small>II</small>)–EDTA by using commercial fluorinated ethylene propylene (FEP) powder as a dielectric catalyst. The reaction generated reactive oxygen species through solid–liquid interfacial charge transfer, disrupting the chemical bonds and then oxidizing the central atoms in Co(<small>II</small>)–EDTA to form Co(<small>III</small>)–EDTA with vacancies. The Co(<small>III</small>)–EDTA could be easily removed from the solution under alkaline conditions. The decomplexation efficiency reached a high value of 41.6%, with a constant reaction rate of 0.024 min<small><sup>−1</sup></small> in 240 minutes. The FEP also exhibited excellent recyclability over 40 h without obvious changes. Unlike conventional advanced oxidation processes, this approach does not require the use of electrodes or chemical oxidants, leading to low energy consumption. This approach also holds great potential for green wastewater management <em>via</em> integration with ambient mechanical energy sources (<em>e.g.</em>, wind and hydrostatic pressure).</p>\",\"PeriodicalId\":99,\"journal\":{\"name\":\"Physical Chemistry Chemical Physics\",\"volume\":\" 29\",\"pages\":\" 15742-15748\"},\"PeriodicalIF\":2.9000,\"publicationDate\":\"2025-07-04\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Physical Chemistry Chemical Physics\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.rsc.org/en/content/articlelanding/2025/cp/d5cp01566a\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Physical Chemistry Chemical Physics","FirstCategoryId":"92","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2025/cp/d5cp01566a","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Promoting Co(ii)–EDTA decomplexation by central atom oxidation in contact-electro-catalysis†
Low-level radioactive wastewater containing Co(II)–EDTA generated in the nuclear industry is harmful to the environment, but it is difficult to remove owing to the high stability of metal–organic complexes. Here, we report efficient contact-electro-catalysis (CEC) to achieve the decomplexation of Co(II)–EDTA by using commercial fluorinated ethylene propylene (FEP) powder as a dielectric catalyst. The reaction generated reactive oxygen species through solid–liquid interfacial charge transfer, disrupting the chemical bonds and then oxidizing the central atoms in Co(II)–EDTA to form Co(III)–EDTA with vacancies. The Co(III)–EDTA could be easily removed from the solution under alkaline conditions. The decomplexation efficiency reached a high value of 41.6%, with a constant reaction rate of 0.024 min−1 in 240 minutes. The FEP also exhibited excellent recyclability over 40 h without obvious changes. Unlike conventional advanced oxidation processes, this approach does not require the use of electrodes or chemical oxidants, leading to low energy consumption. This approach also holds great potential for green wastewater management via integration with ambient mechanical energy sources (e.g., wind and hydrostatic pressure).
期刊介绍:
Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions.
The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.