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

IF 5.1 3区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Nanoscale Pub Date : 2025-10-09 DOI:10.1039/d5nr03230j
Longhuan Dai, Xinlong Yan, Rui Feng, Tianbo Li, Feifei Yang, Xiaoyan Hu, Fei Wei, Yuan Bai, Mengqing Hu
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引用次数: 0

摘要

纳米结构铁基催化剂因其在非均相Fenton反应中降解有机污染物的应用而受到广泛关注。然而,这些催化剂在氧化条件下往往表现出有限的活性和稳定性。本研究采用碳辅助闪蒸焦耳加热(FJH)方法合成了一种新型石墨碳包封Fe/Fe3N/FeN催化剂(Fe- nc -FJH)。该催化剂被专门设计用于激活过氧单硫酸根(PMS)有效降解喹啉,并阐明了其催化活性的基本机制。实验结果表明,Fe-NC-FJH的降解效率显著提高,拟一级降解反应动力学速率(k = 0.18 min−1)比传统热解方法制备的催化剂高2.14倍。密度泛函理论计算表明,石墨碳包封增强了Fe-NC-FJH对PMS羟基O原子的吸附,从而提高了有机矿化至关重要的SO4•−自由基的产率。此外,Fe-NC-FJH在较宽的pH范围内(~ 3-11)表现出强大的催化活性,并且在连续三个循环中表现出显著的降解性能稳定性。最后,提出了喹啉的三种降解途径,包括22种中间体。使用定量构效关系(QSAR)分析对这些中间体的毒性进行了评估,为深入了解高级氧化过程的环境影响提供了有价值的见解。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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.
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来源期刊
Nanoscale
Nanoscale CHEMISTRY, MULTIDISCIPLINARY-NANOSCIENCE & NANOTECHNOLOGY
CiteScore
12.10
自引率
3.00%
发文量
1628
审稿时长
1.6 months
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.
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