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Efficient catalytic wet oxidation of phenol using iron acetylacetonate complexes anchored on carbon nanofibres

机译:使用锚定在碳纳米纤维上的乙酰丙酮铁络合物高效催化湿式氧化苯酚

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摘要

Iron acetylacetonate complexes anchored on oxidized carbon nanofibres (CNFs) were prepared by a three steps procedure: (i) oxidation of commercial CNFs by treatment with HNO3, (ii) synthesis of acetylacetonate (acac) functional groups on the oxidized CNFs surfaces (acac/CNFs) and (iii) iron ions complexation on the acac sites of the CNFs (Fe-acac/ CNFs). The surface groups exposed on the functionalized CNFs were characterized by using attenuated total reflectance Fourier transform infrared spectroscopy, temperature programmed desorption, thermogravimetric analysis and X-ray photoelectron spectroscopy. The functionalized CNFs and the iron complexes anchored on the CNFs were tested as heterogeneous catalysts for the wet oxidation of phenol with pure oxygen. Complete phenol conversion and high mineralization values were achieved with fresh and reused Fe-acac/ CNFs catalysts, which demonstrate the improved stability of the catalysts under the phenol degradation reaction conditions. Furthermore these conditions are comparatively mild, typically 413 K of reaction temperature and 2.0 MPa of oxygen pressure.
机译:通过三个步骤制备锚定在氧化碳纳米纤维(CNF)上的乙酰丙酮铁络合物:(i)通过用HNO3处理氧化商业CNF,(ii)在氧化的CNF表面上合成乙酰丙酮(acac)官能团(acac / CNFs)和(iii)铁离子在CNFs(Fe-acac / CNFs)的acac位点上的络合。通过使用衰减全反射傅里叶变换红外光谱,程序升温解吸,热重分析和X射线光电子能谱,对功能化CNF上暴露的表面基团进行了表征。测试了官能化的CNF和锚定在CNF上的铁络合物作为非均相催化剂用于苯酚与纯氧的湿式氧化。使用新鲜和重复使用的Fe-acac / CNFs催化剂可实现完全的苯酚转化和高矿化值,这表明在苯酚降解反应条件下,催化剂的稳定性得到了提高。此外,这些条件相对温和,通常反应温度为413 K,氧气压力为2.0 MPa。

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