Yunze Wang, Yuan Pan, Xiansheng Zhang, Xinyi Huang, Teng Li, Sheng Liu, Shanqing Tang, Yuanyuan Sun, Binbin Shao, Zhifeng Liu
{"title":"通过缺陷工程提高多酞菁钴的 PMS 活化活性:促进 Co(IV)=O 的形成并提高 1O2 的选择性","authors":"Yunze Wang, Yuan Pan, Xiansheng Zhang, Xinyi Huang, Teng Li, Sheng Liu, Shanqing Tang, Yuanyuan Sun, Binbin Shao, Zhifeng Liu","doi":"10.1016/j.seppur.2024.130085","DOIUrl":null,"url":null,"abstract":"The use of unsaturated Co-N<sub>4</sub> coordinated cobalt polyphthalocyanine (CoPPc) in activating peroxymonosulfate (PMS) for the degradation of organic pollutants has potential applications, but the π-π stacking structure limits the axial electron transfer, hindering the activation of PMS. In this research, a simple hydrothermal modification method was proposed to introduce structural defects into CoPPc. Structural defects can serve as channels for axial electron transfer, which not only reduces the electron transfer resistance but also lowers the oxidation–reduction potential of the central Co ion, favoring the formation of high-valent metal-oxo species (Co(Ⅳ)=O). Additionally, the formation of graphitic carbon, graphitic N, and carbonyl groups during the modification of defective cobalt polyphthalocyanine (D-CoPPc) enhances the selectivity of generating singlet oxygen (<sup>1</sup>O<sub>2</sub>) during the activation of PMS. Therefore, the degradation efficiency of tetracycline (TC) in the D-CoPPc/PMS system, with dual non-radicals (Co(Ⅳ)=O and <sup>1</sup>O<sub>2</sub>) as the main pathway and <span><math><msubsup is=\"true\"><mtext is=\"true\">SO</mtext><mrow is=\"true\"><mtext is=\"true\">4</mtext></mrow><mrow is=\"true\"><mo is=\"true\">·</mo><mo is=\"true\">-</mo></mrow></msubsup></math></span> as auxiliary pathway, increased from 68.0 % to 95.9 %. The outcomes of the experiment demonstrated that D-CoPPc/PMS is also feasible for withstanding natural water bodies, pH variations, and the interference of anions. This study provides new insights into the modification of cobalt polyphthalocyanine and proves its huge potential in organic pollutant degradation.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":null,"pages":null},"PeriodicalIF":8.1000,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Defect engineering boosting PMS activation activity on cobalt polyphthalocyanine: Promoting Co(IV)=O formation and enhancing 1O2 selectivity\",\"authors\":\"Yunze Wang, Yuan Pan, Xiansheng Zhang, Xinyi Huang, Teng Li, Sheng Liu, Shanqing Tang, Yuanyuan Sun, Binbin Shao, Zhifeng Liu\",\"doi\":\"10.1016/j.seppur.2024.130085\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The use of unsaturated Co-N<sub>4</sub> coordinated cobalt polyphthalocyanine (CoPPc) in activating peroxymonosulfate (PMS) for the degradation of organic pollutants has potential applications, but the π-π stacking structure limits the axial electron transfer, hindering the activation of PMS. In this research, a simple hydrothermal modification method was proposed to introduce structural defects into CoPPc. Structural defects can serve as channels for axial electron transfer, which not only reduces the electron transfer resistance but also lowers the oxidation–reduction potential of the central Co ion, favoring the formation of high-valent metal-oxo species (Co(Ⅳ)=O). Additionally, the formation of graphitic carbon, graphitic N, and carbonyl groups during the modification of defective cobalt polyphthalocyanine (D-CoPPc) enhances the selectivity of generating singlet oxygen (<sup>1</sup>O<sub>2</sub>) during the activation of PMS. Therefore, the degradation efficiency of tetracycline (TC) in the D-CoPPc/PMS system, with dual non-radicals (Co(Ⅳ)=O and <sup>1</sup>O<sub>2</sub>) as the main pathway and <span><math><msubsup is=\\\"true\\\"><mtext is=\\\"true\\\">SO</mtext><mrow is=\\\"true\\\"><mtext is=\\\"true\\\">4</mtext></mrow><mrow is=\\\"true\\\"><mo is=\\\"true\\\">·</mo><mo is=\\\"true\\\">-</mo></mrow></msubsup></math></span> as auxiliary pathway, increased from 68.0 % to 95.9 %. The outcomes of the experiment demonstrated that D-CoPPc/PMS is also feasible for withstanding natural water bodies, pH variations, and the interference of anions. This study provides new insights into the modification of cobalt polyphthalocyanine and proves its huge potential in organic pollutant degradation.\",\"PeriodicalId\":427,\"journal\":{\"name\":\"Separation and Purification Technology\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":8.1000,\"publicationDate\":\"2024-10-11\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Separation and Purification Technology\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://doi.org/10.1016/j.seppur.2024.130085\",\"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":"Separation and Purification Technology","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1016/j.seppur.2024.130085","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}
Defect engineering boosting PMS activation activity on cobalt polyphthalocyanine: Promoting Co(IV)=O formation and enhancing 1O2 selectivity
The use of unsaturated Co-N4 coordinated cobalt polyphthalocyanine (CoPPc) in activating peroxymonosulfate (PMS) for the degradation of organic pollutants has potential applications, but the π-π stacking structure limits the axial electron transfer, hindering the activation of PMS. In this research, a simple hydrothermal modification method was proposed to introduce structural defects into CoPPc. Structural defects can serve as channels for axial electron transfer, which not only reduces the electron transfer resistance but also lowers the oxidation–reduction potential of the central Co ion, favoring the formation of high-valent metal-oxo species (Co(Ⅳ)=O). Additionally, the formation of graphitic carbon, graphitic N, and carbonyl groups during the modification of defective cobalt polyphthalocyanine (D-CoPPc) enhances the selectivity of generating singlet oxygen (1O2) during the activation of PMS. Therefore, the degradation efficiency of tetracycline (TC) in the D-CoPPc/PMS system, with dual non-radicals (Co(Ⅳ)=O and 1O2) as the main pathway and as auxiliary pathway, increased from 68.0 % to 95.9 %. The outcomes of the experiment demonstrated that D-CoPPc/PMS is also feasible for withstanding natural water bodies, pH variations, and the interference of anions. This study provides new insights into the modification of cobalt polyphthalocyanine and proves its huge potential in organic pollutant degradation.
期刊介绍:
Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.