{"title":"自芬顿级联反应中的铁、氮掺杂碳点/荧光粉:改进的光降解机制和毒性评估","authors":"","doi":"10.1016/j.jece.2024.114151","DOIUrl":null,"url":null,"abstract":"<div><p>The nanozyme, identified among the top ten emerging technologies in chemistry, has shown rapid development in nano-catalysis for tumour treatment, particularly through its Fenton-like reaction. Herein, a novel iron, nitrogen-doped carbon dots (Fe, N-CDs) with nanozyme catalytic properties was designed, which was then surface-modified onto resorcinol-formaldehyde (RF) resin. Subsequently, a heterogeneous photo-Fenton-like cascade system was constructed to produce and activate photo-generated hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) in situ. Within a broad pH range of 5–9, Fe, N-CDs/RF composites demonstrated superior photocatalytic activity compared to RF alone. Under visible light irradiation, degradation of chloroquine phosphate (CQ) was achieved with a degradation rate constant (k) 3.2 times higher than that observed for RF. Active species capture experiments revealed that hydroxyl radicals (•OH) and superoxide radicals (•O<sub>2</sub><sup>-</sup>) are crucial in propelling the photocatalytic reaction. Furthermore, Density Functional Theory (DFT) calculations indicated that introduction of nanozymes enhances the transfer of electrons from RF surfaces to Fe, N-CDs, high adsorption ability of Fe, N-CDs towards H<sub>2</sub>O<sub>2</sub> (E<sub>ads</sub>=-5.45 eV) in the Fe, N-CDs/RF composites was exploited, thereby augmenting their photocatalytic activity. The possible degradation mechanism of CQ was proposed, and environmental toxicity of CQ degradation intermediates was assessed by seed experiments. This study extends the application scope of carbon dot nanozymes in self-sufficient photo-Fenton systems.</p></div>","PeriodicalId":15759,"journal":{"name":"Journal of Environmental Chemical Engineering","volume":null,"pages":null},"PeriodicalIF":7.4000,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Fe, N-doped carbon dots/RF in self-Fenton cascade reaction: Improved photodegradation mechanism and toxicity evaluation\",\"authors\":\"\",\"doi\":\"10.1016/j.jece.2024.114151\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>The nanozyme, identified among the top ten emerging technologies in chemistry, has shown rapid development in nano-catalysis for tumour treatment, particularly through its Fenton-like reaction. Herein, a novel iron, nitrogen-doped carbon dots (Fe, N-CDs) with nanozyme catalytic properties was designed, which was then surface-modified onto resorcinol-formaldehyde (RF) resin. Subsequently, a heterogeneous photo-Fenton-like cascade system was constructed to produce and activate photo-generated hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) in situ. Within a broad pH range of 5–9, Fe, N-CDs/RF composites demonstrated superior photocatalytic activity compared to RF alone. Under visible light irradiation, degradation of chloroquine phosphate (CQ) was achieved with a degradation rate constant (k) 3.2 times higher than that observed for RF. Active species capture experiments revealed that hydroxyl radicals (•OH) and superoxide radicals (•O<sub>2</sub><sup>-</sup>) are crucial in propelling the photocatalytic reaction. Furthermore, Density Functional Theory (DFT) calculations indicated that introduction of nanozymes enhances the transfer of electrons from RF surfaces to Fe, N-CDs, high adsorption ability of Fe, N-CDs towards H<sub>2</sub>O<sub>2</sub> (E<sub>ads</sub>=-5.45 eV) in the Fe, N-CDs/RF composites was exploited, thereby augmenting their photocatalytic activity. The possible degradation mechanism of CQ was proposed, and environmental toxicity of CQ degradation intermediates was assessed by seed experiments. This study extends the application scope of carbon dot nanozymes in self-sufficient photo-Fenton systems.</p></div>\",\"PeriodicalId\":15759,\"journal\":{\"name\":\"Journal of Environmental Chemical Engineering\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":7.4000,\"publicationDate\":\"2024-09-16\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Environmental Chemical Engineering\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2213343724022826\",\"RegionNum\":2,\"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":"Journal of Environmental Chemical Engineering","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2213343724022826","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Fe, N-doped carbon dots/RF in self-Fenton cascade reaction: Improved photodegradation mechanism and toxicity evaluation
The nanozyme, identified among the top ten emerging technologies in chemistry, has shown rapid development in nano-catalysis for tumour treatment, particularly through its Fenton-like reaction. Herein, a novel iron, nitrogen-doped carbon dots (Fe, N-CDs) with nanozyme catalytic properties was designed, which was then surface-modified onto resorcinol-formaldehyde (RF) resin. Subsequently, a heterogeneous photo-Fenton-like cascade system was constructed to produce and activate photo-generated hydrogen peroxide (H2O2) in situ. Within a broad pH range of 5–9, Fe, N-CDs/RF composites demonstrated superior photocatalytic activity compared to RF alone. Under visible light irradiation, degradation of chloroquine phosphate (CQ) was achieved with a degradation rate constant (k) 3.2 times higher than that observed for RF. Active species capture experiments revealed that hydroxyl radicals (•OH) and superoxide radicals (•O2-) are crucial in propelling the photocatalytic reaction. Furthermore, Density Functional Theory (DFT) calculations indicated that introduction of nanozymes enhances the transfer of electrons from RF surfaces to Fe, N-CDs, high adsorption ability of Fe, N-CDs towards H2O2 (Eads=-5.45 eV) in the Fe, N-CDs/RF composites was exploited, thereby augmenting their photocatalytic activity. The possible degradation mechanism of CQ was proposed, and environmental toxicity of CQ degradation intermediates was assessed by seed experiments. This study extends the application scope of carbon dot nanozymes in self-sufficient photo-Fenton systems.
期刊介绍:
The Journal of Environmental Chemical Engineering (JECE) serves as a platform for the dissemination of original and innovative research focusing on the advancement of environmentally-friendly, sustainable technologies. JECE emphasizes the transition towards a carbon-neutral circular economy and a self-sufficient bio-based economy. Topics covered include soil, water, wastewater, and air decontamination; pollution monitoring, prevention, and control; advanced analytics, sensors, impact and risk assessment methodologies in environmental chemical engineering; resource recovery (water, nutrients, materials, energy); industrial ecology; valorization of waste streams; waste management (including e-waste); climate-water-energy-food nexus; novel materials for environmental, chemical, and energy applications; sustainability and environmental safety; water digitalization, water data science, and machine learning; process integration and intensification; recent developments in green chemistry for synthesis, catalysis, and energy; and original research on contaminants of emerging concern, persistent chemicals, and priority substances, including microplastics, nanoplastics, nanomaterials, micropollutants, antimicrobial resistance genes, and emerging pathogens (viruses, bacteria, parasites) of environmental significance.