Two-dimensional graphene oxide-iron oxide catalysts for oxidation of sulfides: Synthesis, product analysis, and environmental impact

IF 4 2区 化学 Q2 CHEMISTRY, PHYSICAL
Amanda Ineza Mugisha , Clémence Fauteux-Lefebvre , Pandiyan Thangarasu , Carlos Alberto Huerta-Aguilar
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Abstract

The efficient and sustainable oxidation of organic sulfides is crucial for environmental remediation and the production of specialty chemicals. The unique molecular structure of two-dimensional graphene oxide (GO) enables its application in environmental catalysis, particularly when combined with active metal oxides. This study presents a sustainable synthesis of GO-Fe₃O₄ composites via co-precipitation and wet-deposition methods, forming 15 nm iron oxide nanoparticles uniformly anchored on 200 nm GO sheets. Characterization by TEM, XRD, and FTIR confirmed the crystalline structure and successful integration of Fe₃O₄ onto GO. The composite achieved a thioanisole conversion of 95.8 % in the presence of H₂O₂ and 64.2 % without H₂O₂, under mild conditions (50 °C, 5 h). Photocatalytic studies demonstrated conversions of 89.6 %, 77.7 %, and 75.2 % under UV, sunlight, and visible light, respectively, with a direct band gap reduction from 3.23 eV (GO) to 2.24 eV (GO-Fe₃O₄). These results highlight the interplay of GO's electron mobility and Fe₃O₄ catalytic activity in generating reactive oxygen species (•OH and O₂•⁻) through Fenton and photocatalytic processes. Furthermore, energy and environmental assessments revealed that the synthesis method required only 24.79 kWh/g of catalyst, with a total emission of 10.32 kgCO₂/g catalyst, emphasizing its low carbon footprint and material efficiency. Additionally, this work provides mechanistic insights into the synergistic interactions between GO and Fe₃O₄, advancing the design of 2D carbon-based materials for sustainable sulfur removal and green chemical applications.

Abstract Image

用于硫化物氧化的二维氧化石墨烯-氧化铁催化剂:合成,产品分析和环境影响
有机硫化物的高效、可持续氧化对环境修复和特种化学品生产至关重要。二维氧化石墨烯(GO)独特的分子结构使其能够应用于环境催化,特别是当与活性金属氧化物结合时。采用共沉淀法和湿沉积法合成了GO- fe₃O₄复合材料,在200 nm的氧化石墨烯薄片上形成了15 nm的氧化铁纳米颗粒。TEM、XRD和FTIR表征证实了Fe₃O₄在氧化石墨烯上的成功整合。在温和条件下(50°C, 5 H),该复合材料在h2₂O₂存在下的硫代苯甲醚转化率为95.8%,在无h2₂O₂存在下的转化率为64.2%。光催化研究表明,在紫外线、阳光和可见光下的转化率分别为89.6%、77.7%和75.2%,直接带隙从3.23 eV (GO- fe₃O₄)降低到2.24 eV (GO- fe₃O₄)。这些结果强调了氧化石墨烯的电子迁移率和Fe₃O₄催化活性在通过Fenton和光催化过程产生活性氧(•OH和O₂•⁻)中的相互作用。此外,能源和环境评价表明,该合成方法只需要24.79 kWh/g催化剂,催化剂总排放量为10.32 kgCO₂/g,强调其低碳足迹和材料效率。此外,这项工作为氧化石墨烯和Fe₃O₄之间的协同相互作用提供了机理见解,推进了二维碳基材料的设计,用于可持续除硫和绿色化学应用。
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来源期刊
Journal of Molecular Structure
Journal of Molecular Structure 化学-物理化学
CiteScore
7.10
自引率
15.80%
发文量
2384
审稿时长
45 days
期刊介绍: The Journal of Molecular Structure is dedicated to the publication of full-length articles and review papers, providing important new structural information on all types of chemical species including: • Stable and unstable molecules in all types of environments (vapour, molecular beam, liquid, solution, liquid crystal, solid state, matrix-isolated, surface-absorbed etc.) • Chemical intermediates • Molecules in excited states • Biological molecules • Polymers. The methods used may include any combination of spectroscopic and non-spectroscopic techniques, for example: • Infrared spectroscopy (mid, far, near) • Raman spectroscopy and non-linear Raman methods (CARS, etc.) • Electronic absorption spectroscopy • Optical rotatory dispersion and circular dichroism • Fluorescence and phosphorescence techniques • Electron spectroscopies (PES, XPS), EXAFS, etc. • Microwave spectroscopy • Electron diffraction • NMR and ESR spectroscopies • Mössbauer spectroscopy • X-ray crystallography • Charge Density Analyses • Computational Studies (supplementing experimental methods) We encourage publications combining theoretical and experimental approaches. The structural insights gained by the studies should be correlated with the properties, activity and/ or reactivity of the molecule under investigation and the relevance of this molecule and its implications should be discussed.
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