{"title":"石墨碳包封Fe/ fe3n /FeN催化剂的焦耳热合成及其对喹啉的高效过氧单硫酸盐活化","authors":"Longhuan Dai, Xinlong Yan, Rui Feng, Tianbo Li, Feifei Yang, Xiaoyan Hu, Fei Wei, Yuan Bai, Mengqing Hu","doi":"10.1039/d5nr03230j","DOIUrl":null,"url":null,"abstract":"Nanostructured iron-based catalysts have garnered significant attention for their application in heterogeneous Fenton reactions aimed at organic pollutant degradation. However, these catalysts often exhibit limited activity and stability under oxidation conditions. In this study, a novel graphitic carbon-encapsulated Fe/Fe3N/FeN catalyst (Fe-NC-FJH) was synthesized using a carbon-assisted flash Joule heating (FJH) method. The catalyst was specifically engineered to activate peroxymonosulfate (PMS) for effective quinoline degradation, with the fundamental mechanisms governing its catalytic activity being elucidated. Experimental results demonstrated that Fe-NC-FJH displayed significantly enhanced degradation efficiency and a higher pseudo-first-order degradation reaction kinetic rate (k = 0.18 min−1), which was 2.14 times greater than that achieved by catalysts prepared using conventional pyrolysis methods. Density functional theory calculations suggested that the graphitic carbon encapsulation enhanced the adsorption of Fe-NC-FJH for the hydroxyl O atom of PMS, thereby increasing the yield of SO4•− radicals crucial for organic mineralization. Furthermore, Fe-NC-FJH exhibited robust catalytic activity across a broad pH range (~3–11) and demonstrated remarkable stability in degradation performance over three consecutive cycles. Lastly, three degradation pathways of Quinoline, encompassing 22 intermediates, were proposed. The toxicity of these intermediates was evaluated using quantitative structure–activity relationship (QSAR) analysis, providing valuable insights into the environmental impact of the advanced oxidation process.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"21 1","pages":""},"PeriodicalIF":5.1000,"publicationDate":"2025-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Joule-Thermal Synthesis of Graphitic Carbon-Encapsulated Fe/Fe 3 N/FeN Catalysts for Efficient Peroxymonosulfate Activation toward Quinoline Degradation\",\"authors\":\"Longhuan Dai, Xinlong Yan, Rui Feng, Tianbo Li, Feifei Yang, Xiaoyan Hu, Fei Wei, Yuan Bai, Mengqing Hu\",\"doi\":\"10.1039/d5nr03230j\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Nanostructured iron-based catalysts have garnered significant attention for their application in heterogeneous Fenton reactions aimed at organic pollutant degradation. However, these catalysts often exhibit limited activity and stability under oxidation conditions. In this study, a novel graphitic carbon-encapsulated Fe/Fe3N/FeN catalyst (Fe-NC-FJH) was synthesized using a carbon-assisted flash Joule heating (FJH) method. The catalyst was specifically engineered to activate peroxymonosulfate (PMS) for effective quinoline degradation, with the fundamental mechanisms governing its catalytic activity being elucidated. Experimental results demonstrated that Fe-NC-FJH displayed significantly enhanced degradation efficiency and a higher pseudo-first-order degradation reaction kinetic rate (k = 0.18 min−1), which was 2.14 times greater than that achieved by catalysts prepared using conventional pyrolysis methods. Density functional theory calculations suggested that the graphitic carbon encapsulation enhanced the adsorption of Fe-NC-FJH for the hydroxyl O atom of PMS, thereby increasing the yield of SO4•− radicals crucial for organic mineralization. Furthermore, Fe-NC-FJH exhibited robust catalytic activity across a broad pH range (~3–11) and demonstrated remarkable stability in degradation performance over three consecutive cycles. Lastly, three degradation pathways of Quinoline, encompassing 22 intermediates, were proposed. The toxicity of these intermediates was evaluated using quantitative structure–activity relationship (QSAR) analysis, providing valuable insights into the environmental impact of the advanced oxidation process.\",\"PeriodicalId\":92,\"journal\":{\"name\":\"Nanoscale\",\"volume\":\"21 1\",\"pages\":\"\"},\"PeriodicalIF\":5.1000,\"publicationDate\":\"2025-10-09\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Nanoscale\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1039/d5nr03230j\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nanoscale","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1039/d5nr03230j","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Joule-Thermal Synthesis of Graphitic Carbon-Encapsulated Fe/Fe 3 N/FeN Catalysts for Efficient Peroxymonosulfate Activation toward Quinoline Degradation
Nanostructured iron-based catalysts have garnered significant attention for their application in heterogeneous Fenton reactions aimed at organic pollutant degradation. However, these catalysts often exhibit limited activity and stability under oxidation conditions. In this study, a novel graphitic carbon-encapsulated Fe/Fe3N/FeN catalyst (Fe-NC-FJH) was synthesized using a carbon-assisted flash Joule heating (FJH) method. The catalyst was specifically engineered to activate peroxymonosulfate (PMS) for effective quinoline degradation, with the fundamental mechanisms governing its catalytic activity being elucidated. Experimental results demonstrated that Fe-NC-FJH displayed significantly enhanced degradation efficiency and a higher pseudo-first-order degradation reaction kinetic rate (k = 0.18 min−1), which was 2.14 times greater than that achieved by catalysts prepared using conventional pyrolysis methods. Density functional theory calculations suggested that the graphitic carbon encapsulation enhanced the adsorption of Fe-NC-FJH for the hydroxyl O atom of PMS, thereby increasing the yield of SO4•− radicals crucial for organic mineralization. Furthermore, Fe-NC-FJH exhibited robust catalytic activity across a broad pH range (~3–11) and demonstrated remarkable stability in degradation performance over three consecutive cycles. Lastly, three degradation pathways of Quinoline, encompassing 22 intermediates, were proposed. The toxicity of these intermediates was evaluated using quantitative structure–activity relationship (QSAR) analysis, providing valuable insights into the environmental impact of the advanced oxidation process.
期刊介绍:
Nanoscale is a high-impact international journal, publishing high-quality research across nanoscience and nanotechnology. Nanoscale publishes a full mix of research articles on experimental and theoretical work, including reviews, communications, and full papers.Highly interdisciplinary, this journal appeals to scientists, researchers and professionals interested in nanoscience and nanotechnology, quantum materials and quantum technology, including the areas of physics, chemistry, biology, medicine, materials, energy/environment, information technology, detection science, healthcare and drug discovery, and electronics.