Dongqi Tian , Shuai Yang , Yang Liu , Hongyu Zhou , Peng Zhou , Zhaokun Xiong , Gang Yao , Bo Lai
{"title":"沸石咪唑框架-8衍生的氮掺杂纳米碳促进类芬顿氧化:Fe(III)/Fe(II)循环的另一条可持续途径","authors":"Dongqi Tian , Shuai Yang , Yang Liu , Hongyu Zhou , Peng Zhou , Zhaokun Xiong , Gang Yao , Bo Lai","doi":"10.1016/j.efmat.2022.10.001","DOIUrl":null,"url":null,"abstract":"<div><p>Zeolite imidazole framework-8 (ZIF-8) is a promising template to obtain porous nanocarbons. In this study, microporous nitrogen-doped nanocarbons from the carbonization of ZIF-8 (ZCN) was prepared as an efficient metal-free catalyst to improve several micropollutants degradation in Fe(III)/H<sub>2</sub>O<sub>2</sub> process. The sulfamethoxazole (SMX) ratio was increased from 20% to 100% with the addition of ZCN (50 mg/L) in Fe(III)/H<sub>2</sub>O<sub>2</sub> within 20 min, and the working pH was endowed. The direct reduction for Fe(III) resulting from carbonyl on ZCN's surface was revealed. Hydroxyl radical (•OH) was determined to be the main reactive species, and the evolution of different Fe species during the reaction was discussed by monitoring the mass balance of Fe species. We found that part of the iron was bound to the surface of ZCN during the reaction. Additionally, the dissociative Fe was captured by ZCN to form Fe-N<sub><em>x</em></sub> bonds. Surface-bound Fe with a lower energy barrier was more likely to react with H<sub>2</sub>O<sub>2</sub> to generate Fe(II). Our work revealed that in addition to the direct reduction by ZCN, another catalytic reduction pathway for the sustainable conversion of Fe(III) to Fe(II) in the ZCN/Fe(III)/H<sub>2</sub>O<sub>2</sub> process was operative.</p></div>","PeriodicalId":100481,"journal":{"name":"Environmental Functional Materials","volume":"1 3","pages":"Pages 267-274"},"PeriodicalIF":0.0000,"publicationDate":"2022-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2773058122000369/pdfft?md5=76c402860a78c769d629db48cadf2aed&pid=1-s2.0-S2773058122000369-main.pdf","citationCount":"0","resultStr":"{\"title\":\"Zeolite imidazole framework-8-derived nitrogen-doped nanocarbon boosted Fenton-like oxidation: Another sustainable path for Fe(III)/Fe(II) circulation\",\"authors\":\"Dongqi Tian , Shuai Yang , Yang Liu , Hongyu Zhou , Peng Zhou , Zhaokun Xiong , Gang Yao , Bo Lai\",\"doi\":\"10.1016/j.efmat.2022.10.001\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Zeolite imidazole framework-8 (ZIF-8) is a promising template to obtain porous nanocarbons. In this study, microporous nitrogen-doped nanocarbons from the carbonization of ZIF-8 (ZCN) was prepared as an efficient metal-free catalyst to improve several micropollutants degradation in Fe(III)/H<sub>2</sub>O<sub>2</sub> process. The sulfamethoxazole (SMX) ratio was increased from 20% to 100% with the addition of ZCN (50 mg/L) in Fe(III)/H<sub>2</sub>O<sub>2</sub> within 20 min, and the working pH was endowed. The direct reduction for Fe(III) resulting from carbonyl on ZCN's surface was revealed. Hydroxyl radical (•OH) was determined to be the main reactive species, and the evolution of different Fe species during the reaction was discussed by monitoring the mass balance of Fe species. We found that part of the iron was bound to the surface of ZCN during the reaction. Additionally, the dissociative Fe was captured by ZCN to form Fe-N<sub><em>x</em></sub> bonds. Surface-bound Fe with a lower energy barrier was more likely to react with H<sub>2</sub>O<sub>2</sub> to generate Fe(II). Our work revealed that in addition to the direct reduction by ZCN, another catalytic reduction pathway for the sustainable conversion of Fe(III) to Fe(II) in the ZCN/Fe(III)/H<sub>2</sub>O<sub>2</sub> process was operative.</p></div>\",\"PeriodicalId\":100481,\"journal\":{\"name\":\"Environmental Functional Materials\",\"volume\":\"1 3\",\"pages\":\"Pages 267-274\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2022-09-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.sciencedirect.com/science/article/pii/S2773058122000369/pdfft?md5=76c402860a78c769d629db48cadf2aed&pid=1-s2.0-S2773058122000369-main.pdf\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Environmental Functional Materials\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2773058122000369\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Environmental Functional Materials","FirstCategoryId":"1085","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2773058122000369","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
Zeolite imidazole framework-8-derived nitrogen-doped nanocarbon boosted Fenton-like oxidation: Another sustainable path for Fe(III)/Fe(II) circulation
Zeolite imidazole framework-8 (ZIF-8) is a promising template to obtain porous nanocarbons. In this study, microporous nitrogen-doped nanocarbons from the carbonization of ZIF-8 (ZCN) was prepared as an efficient metal-free catalyst to improve several micropollutants degradation in Fe(III)/H2O2 process. The sulfamethoxazole (SMX) ratio was increased from 20% to 100% with the addition of ZCN (50 mg/L) in Fe(III)/H2O2 within 20 min, and the working pH was endowed. The direct reduction for Fe(III) resulting from carbonyl on ZCN's surface was revealed. Hydroxyl radical (•OH) was determined to be the main reactive species, and the evolution of different Fe species during the reaction was discussed by monitoring the mass balance of Fe species. We found that part of the iron was bound to the surface of ZCN during the reaction. Additionally, the dissociative Fe was captured by ZCN to form Fe-Nx bonds. Surface-bound Fe with a lower energy barrier was more likely to react with H2O2 to generate Fe(II). Our work revealed that in addition to the direct reduction by ZCN, another catalytic reduction pathway for the sustainable conversion of Fe(III) to Fe(II) in the ZCN/Fe(III)/H2O2 process was operative.