Xiayan Zhang , Zhi Song , Boxia Liu , Bofei Liu , Jialu Liu , Jinrong Lu , Cheng Li , Yeqiong Huang , Dongxu Han , Jingjing Yang , Hua Liu
{"title":"在纳米尺度畴限制和距离效应下,Pr0.6Sm0.4Co0-8Mn0-2O3活化过硫酸盐增强的界面电荷变化被用于高效降解四环素","authors":"Xiayan Zhang , Zhi Song , Boxia Liu , Bofei Liu , Jialu Liu , Jinrong Lu , Cheng Li , Yeqiong Huang , Dongxu Han , Jingjing Yang , Hua Liu","doi":"10.1016/j.mtsust.2024.101044","DOIUrl":null,"url":null,"abstract":"<div><div>In this work, an improved sol-gel method was used to prepare a series of Co-infused PrSmMnO<sub>3</sub> perovskites (Pr<sub>0.6</sub>Sm<sub>0.4</sub>Co<sub>1-X</sub>Mn<sub>X</sub>O<sub>3</sub>, PSCM) to rapidly activate peroxymonosulfate (PMS) for efficient degradation of tetracycline (TC). The experimental results showed that the degradation efficiency of the PSCM-82/PMS system for TC in the pH 2–11 range was close to 100%. The nanoscale domain-limiting and distance effect of PSCM under different activators were discussed, and the catalytic mechanism of the non-radical electron transfer pathway in the PSCM-82/PMS system was proposed. After the optimization of the DFT calculation, it can be seen that the <em>d</em><sub>Co-Mn-Co</sub> range of the PSCM-82 material is 9.8–9.9 Å. The molecular size of PMS is 9.9 Å, which precisely matches the <em>d</em><sub>Co-Mn-Co</sub> range of the material. Moreover, the distance between molecular sizes was relatively minimal, and the interface charge transfer was enhanced by both the confinement and distance effects. This promotes a fast catalytic reaction and an optimal degradation rate. During this process, PMS molecules were adsorbed by the active metal sites on the surface of PSCM-82, resulting in a large amount of interfacial charge transfer. This allows a strong coupling between the PMS and the catalyst, resulting in a reaction surface with high redox potential. According to the results of density functional theory (DFT) calculation, quenching experiment, electron paramagnetic resonance (EPR) experiment and electrochemical research, it can be concluded that the main degradation pathway of TC is realized through the direct electron transfer process.</div></div>","PeriodicalId":18322,"journal":{"name":"Materials Today Sustainability","volume":"28 ","pages":"Article 101044"},"PeriodicalIF":7.1000,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"The interfacial charge change enhanced by Pr0.6Sm0.4Co0·8Mn0·2O3 activated peroxymonosulfate was used for the efficient degradation of tetracycline under the nanoscale domain limiting and distance effect\",\"authors\":\"Xiayan Zhang , Zhi Song , Boxia Liu , Bofei Liu , Jialu Liu , Jinrong Lu , Cheng Li , Yeqiong Huang , Dongxu Han , Jingjing Yang , Hua Liu\",\"doi\":\"10.1016/j.mtsust.2024.101044\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>In this work, an improved sol-gel method was used to prepare a series of Co-infused PrSmMnO<sub>3</sub> perovskites (Pr<sub>0.6</sub>Sm<sub>0.4</sub>Co<sub>1-X</sub>Mn<sub>X</sub>O<sub>3</sub>, PSCM) to rapidly activate peroxymonosulfate (PMS) for efficient degradation of tetracycline (TC). The experimental results showed that the degradation efficiency of the PSCM-82/PMS system for TC in the pH 2–11 range was close to 100%. The nanoscale domain-limiting and distance effect of PSCM under different activators were discussed, and the catalytic mechanism of the non-radical electron transfer pathway in the PSCM-82/PMS system was proposed. After the optimization of the DFT calculation, it can be seen that the <em>d</em><sub>Co-Mn-Co</sub> range of the PSCM-82 material is 9.8–9.9 Å. The molecular size of PMS is 9.9 Å, which precisely matches the <em>d</em><sub>Co-Mn-Co</sub> range of the material. Moreover, the distance between molecular sizes was relatively minimal, and the interface charge transfer was enhanced by both the confinement and distance effects. This promotes a fast catalytic reaction and an optimal degradation rate. During this process, PMS molecules were adsorbed by the active metal sites on the surface of PSCM-82, resulting in a large amount of interfacial charge transfer. This allows a strong coupling between the PMS and the catalyst, resulting in a reaction surface with high redox potential. According to the results of density functional theory (DFT) calculation, quenching experiment, electron paramagnetic resonance (EPR) experiment and electrochemical research, it can be concluded that the main degradation pathway of TC is realized through the direct electron transfer process.</div></div>\",\"PeriodicalId\":18322,\"journal\":{\"name\":\"Materials Today Sustainability\",\"volume\":\"28 \",\"pages\":\"Article 101044\"},\"PeriodicalIF\":7.1000,\"publicationDate\":\"2024-11-12\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Materials Today Sustainability\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2589234724003804\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Materials Today Sustainability","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2589234724003804","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"GREEN & SUSTAINABLE SCIENCE & TECHNOLOGY","Score":null,"Total":0}
The interfacial charge change enhanced by Pr0.6Sm0.4Co0·8Mn0·2O3 activated peroxymonosulfate was used for the efficient degradation of tetracycline under the nanoscale domain limiting and distance effect
In this work, an improved sol-gel method was used to prepare a series of Co-infused PrSmMnO3 perovskites (Pr0.6Sm0.4Co1-XMnXO3, PSCM) to rapidly activate peroxymonosulfate (PMS) for efficient degradation of tetracycline (TC). The experimental results showed that the degradation efficiency of the PSCM-82/PMS system for TC in the pH 2–11 range was close to 100%. The nanoscale domain-limiting and distance effect of PSCM under different activators were discussed, and the catalytic mechanism of the non-radical electron transfer pathway in the PSCM-82/PMS system was proposed. After the optimization of the DFT calculation, it can be seen that the dCo-Mn-Co range of the PSCM-82 material is 9.8–9.9 Å. The molecular size of PMS is 9.9 Å, which precisely matches the dCo-Mn-Co range of the material. Moreover, the distance between molecular sizes was relatively minimal, and the interface charge transfer was enhanced by both the confinement and distance effects. This promotes a fast catalytic reaction and an optimal degradation rate. During this process, PMS molecules were adsorbed by the active metal sites on the surface of PSCM-82, resulting in a large amount of interfacial charge transfer. This allows a strong coupling between the PMS and the catalyst, resulting in a reaction surface with high redox potential. According to the results of density functional theory (DFT) calculation, quenching experiment, electron paramagnetic resonance (EPR) experiment and electrochemical research, it can be concluded that the main degradation pathway of TC is realized through the direct electron transfer process.
期刊介绍:
Materials Today Sustainability is a multi-disciplinary journal covering all aspects of sustainability through materials science.
With a rapidly increasing population with growing demands, materials science has emerged as a critical discipline toward protecting of the environment and ensuring the long term survival of future generations.