Minjie Yu , Yidan Luo , Zugen Liu , Guangying Shi , Mingshan Xue , Xianchuan Xie , Xibao Li
{"title":"铁基mls的氧空位工程用于快速激子解离的光催化","authors":"Minjie Yu , Yidan Luo , Zugen Liu , Guangying Shi , Mingshan Xue , Xianchuan Xie , Xibao Li","doi":"10.1016/j.seppur.2025.132509","DOIUrl":null,"url":null,"abstract":"<div><div>In this work, MIL-53(Fe) with abundant oxygen vacancies (OVs) and Fe<sup>2+</sup>/Fe<sup>3+</sup> sites was successfully prepared by solvothermal treatment. The MIL-53(Fe) after the ethylene glycol (EG) treatment at 150 °C (EM53-150) displayed the best tetracycline (TC) photodegradation rate (94.37%) and reaction rate constant (0.1111 min<sup>-</sup><sup>1</sup>), which were 2.58 (36.56%) and 22.22 (0.0050 min<sup>-</sup><sup>1</sup>) times for MIL-53(Fe), respectively. The appropriate concentration of OVs in EM53-150 can effectively enhance exciton dissociation, inhibit the recombination of photogenerated electron-hole pairs, and regulate the activation of molecular oxygen to form <span><math><mrow><mo>∙</mo><msubsup><mtext>O</mtext><mrow><mtext>2</mtext></mrow><mtext>-</mtext></msubsup></mrow></math></span> through electron transfer. Similarly, the MIL-88B(Fe) and MIL-101(Fe) modified by EG also improved the photodegradation performance. The potential photodegradation pathways of TC were proposed depending on the Fukui index and the detection results of LC-MS. Finally, the mechanism was revealed based on band structures and reactive species. This work provided favorable prospects for the introduction of OVs and Fe<sup>2+</sup>/Fe<sup>3+</sup> sites in Fe-based MILs for boosting exciton dissociation to degrade antibiotics.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"364 ","pages":"Article 132509"},"PeriodicalIF":9.0000,"publicationDate":"2025-03-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Oxygen-vacancy engineering on Fe-based MILs for efficient photocatalysis with rapid exciton dissociation\",\"authors\":\"Minjie Yu , Yidan Luo , Zugen Liu , Guangying Shi , Mingshan Xue , Xianchuan Xie , Xibao Li\",\"doi\":\"10.1016/j.seppur.2025.132509\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>In this work, MIL-53(Fe) with abundant oxygen vacancies (OVs) and Fe<sup>2+</sup>/Fe<sup>3+</sup> sites was successfully prepared by solvothermal treatment. The MIL-53(Fe) after the ethylene glycol (EG) treatment at 150 °C (EM53-150) displayed the best tetracycline (TC) photodegradation rate (94.37%) and reaction rate constant (0.1111 min<sup>-</sup><sup>1</sup>), which were 2.58 (36.56%) and 22.22 (0.0050 min<sup>-</sup><sup>1</sup>) times for MIL-53(Fe), respectively. The appropriate concentration of OVs in EM53-150 can effectively enhance exciton dissociation, inhibit the recombination of photogenerated electron-hole pairs, and regulate the activation of molecular oxygen to form <span><math><mrow><mo>∙</mo><msubsup><mtext>O</mtext><mrow><mtext>2</mtext></mrow><mtext>-</mtext></msubsup></mrow></math></span> through electron transfer. Similarly, the MIL-88B(Fe) and MIL-101(Fe) modified by EG also improved the photodegradation performance. The potential photodegradation pathways of TC were proposed depending on the Fukui index and the detection results of LC-MS. Finally, the mechanism was revealed based on band structures and reactive species. This work provided favorable prospects for the introduction of OVs and Fe<sup>2+</sup>/Fe<sup>3+</sup> sites in Fe-based MILs for boosting exciton dissociation to degrade antibiotics.</div></div>\",\"PeriodicalId\":427,\"journal\":{\"name\":\"Separation and Purification Technology\",\"volume\":\"364 \",\"pages\":\"Article 132509\"},\"PeriodicalIF\":9.0000,\"publicationDate\":\"2025-03-15\",\"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://www.sciencedirect.com/science/article/pii/S1383586625011062\",\"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://www.sciencedirect.com/science/article/pii/S1383586625011062","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}
Oxygen-vacancy engineering on Fe-based MILs for efficient photocatalysis with rapid exciton dissociation
In this work, MIL-53(Fe) with abundant oxygen vacancies (OVs) and Fe2+/Fe3+ sites was successfully prepared by solvothermal treatment. The MIL-53(Fe) after the ethylene glycol (EG) treatment at 150 °C (EM53-150) displayed the best tetracycline (TC) photodegradation rate (94.37%) and reaction rate constant (0.1111 min-1), which were 2.58 (36.56%) and 22.22 (0.0050 min-1) times for MIL-53(Fe), respectively. The appropriate concentration of OVs in EM53-150 can effectively enhance exciton dissociation, inhibit the recombination of photogenerated electron-hole pairs, and regulate the activation of molecular oxygen to form through electron transfer. Similarly, the MIL-88B(Fe) and MIL-101(Fe) modified by EG also improved the photodegradation performance. The potential photodegradation pathways of TC were proposed depending on the Fukui index and the detection results of LC-MS. Finally, the mechanism was revealed based on band structures and reactive species. This work provided favorable prospects for the introduction of OVs and Fe2+/Fe3+ sites in Fe-based MILs for boosting exciton dissociation to degrade antibiotics.
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.