Farhadi Saeed, Hakimi Mohammad, Maleki Mansoureh
Chemistry Department, Lorestan University Khorramabad 68151-44316 Iran
Chemistry Department, Payame Noor University Tehran 19395-4697 Iran.
RSC Adv. 2018 Feb 12;8(13):6768-6780. doi: 10.1039/c8ra00312b. eCollection 2018 Feb 9.
In this work, 12-molybdophosphoric acid (HPMoO, HPMo) was chemically anchored onto the surface of aminosilanized magnetic graphene oxide (FeO/GrOSi(CH)-NH) and was characterized using different physicochemical techniques, such as powder X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), Raman spectroscopy, energy-dispersive X-ray analysis (EDX), scanning electron microscopy (SEM), BET specific surface area analysis and magnetic measurements. The results demonstrated the successful loading of HPMo (∼31.5 wt%) on the surface of magnetic aminosilanized graphene oxide. XRD patterns, N adsorption-desorption isotherms and SEM images confirm the mesostructure of the sample. FT-IR and EDX spectra indicate the presence of the PMoO polyanions in the nanocomposite. The as-prepared FeO/GrOSi(CH)-NH/HPMo nanocomposite has a specific surface area of 76.36 m g that is much higher than that of pure HPMo. The selective oxidation of benzyl alcohol to benzaldehyde was initially studied as a benchmark reaction to evaluate the catalytic performance of the FeO/GrOSi(CH)-NH/HPMo catalyst. Then, the oxidation of a variety of substituted primary and secondary activated benzylic alcohols was evaluated with HO under solvent-free conditions. Under the optimized conditions, all alcohols were converted into the corresponding aldehydes and ketones with very high selectivity (≥99%) in moderate to excellent yields (60-96%). The high catalytic performance of the nanocomposite was ascribed to its higher specific surface area and more efficient electron transfer, probably due to the presence of GrO nanosheets. The nanocomposite catalyst is readily recovered from the reaction mixture by a usual magnet and reused at least four times without any observable change in structure and catalytic activity.
在本工作中,将12 - 钼磷酸(HPMoO,HPMo)化学锚定在氨基硅烷化磁性氧化石墨烯(FeO/GrOSi(CH)-NH)表面,并使用粉末X射线衍射(XRD)、傅里叶变换红外光谱(FT - IR)、拉曼光谱、能量色散X射线分析(EDX)、扫描电子显微镜(SEM)、BET比表面积分析和磁性测量等不同的物理化学技术对其进行表征。结果表明HPMo(约31.5 wt%)成功负载在磁性氨基硅烷化氧化石墨烯表面。XRD图谱、N吸附 - 解吸等温线和SEM图像证实了样品的介观结构。FT - IR和EDX光谱表明纳米复合材料中存在PMoO多阴离子。所制备的FeO/GrOSi(CH)-NH/HPMo纳米复合材料的比表面积为76.36 m²/g,远高于纯HPMo。最初研究了苯甲醇选择性氧化为苯甲醛作为基准反应,以评估FeO/GrOSi(CH)-NH/HPMo催化剂的催化性能。然后,在无溶剂条件下用H₂O₂评估了各种取代的伯醇和仲醇的氧化反应。在优化条件下,所有醇都以非常高的选择性(≥99%)转化为相应的醛和酮,产率适中至优异(60 - 96%)。纳米复合材料的高催化性能归因于其较高的比表面积和更有效的电子转移,这可能是由于GrO纳米片的存在。纳米复合催化剂很容易通过普通磁铁从反应混合物中回收,并至少重复使用四次,其结构和催化活性没有任何明显变化。