首页> 外文期刊>RSC Advances >12-Molybdophosphoric acid anchored on aminopropylsilanized magnetic graphene oxide nanosheets (Fe3O4/GrOSi(CH2)3–NH2/H3PMo12O40): a novel magnetically recoverable solid catalyst for H2O2-mediated oxidation of benzylic alcohols under solvent-free conditions
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12-Molybdophosphoric acid anchored on aminopropylsilanized magnetic graphene oxide nanosheets (Fe3O4/GrOSi(CH2)3–NH2/H3PMo12O40): a novel magnetically recoverable solid catalyst for H2O2-mediated oxidation of benzylic alcohols under solvent-free conditions

机译:锚固在氨基丙基硅烷化的氧化石墨烯纳米片(Fe3O4 / GrOSi(CH2)3-NH2 / H3PMo12O40)上的12-钼磷酸:无溶剂条件下H2O2介导的苄醇氧化的新型磁性可回收固体催化剂

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In this work, 12-molybdophosphoric acid (H _(3) PMo _(12) O _(40) , HPMo) was chemically anchored onto the surface of aminosilanized magnetic graphene oxide (Fe _(3) O _(4) /GrOSi(CH _(2) ) _(3) –NH _(2) ) 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 _(2) adsorption–desorption isotherms and SEM images confirm the mesostructure of the sample. FT-IR and EDX spectra indicate the presence of the PMo _(12) O _(40) ~(3?) polyanions in the nanocomposite. The as-prepared Fe _(3) O _(4) /GrOSi(CH _(2) ) _(3) –NH _(2) /HPMo nanocomposite has a specific surface area of 76.36 m ~(2) g ~(?1) 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 Fe _(3) O _(4) /GrOSi(CH _(2) ) _(3) –NH _(2) /HPMo catalyst. Then, the oxidation of a variety of substituted primary and secondary activated benzylic alcohols was evaluated with H _(2) O _(2) 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.
机译:在这项工作中,将12钼磷酸(H _(3)PMo _(12)O _(40),HPMo)化学固定在氨基硅烷化磁性氧化石墨烯(Fe _(3)O _(4)/ GrOSi(CH _(2)_(3)-NH _(2)),并使用不同的物理化学技术进行了表征,例如粉末X射线衍射(XRD),傅立叶变换红外光谱(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比表面积分析和磁测量。结果表明,HPMo(〜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 _(2)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光谱表明在纳米复合物中存在PMo_(12)O_(40)〜(3′)聚阴离子。制备的Fe _(3)O _(4)/ GrOSi(CH _(2))_(3)–NH _(2)/ HPMo纳米复合材料的比表面积为76.36 m〜(2)g〜 (?1)比纯HPMo高得多。初步研究了将苄醇选择性氧化为苯甲醛作为基准反应,以评估Fe _(3)O _(4)/ GrOSi(CH _(2))_(3)-NH _(2 )/ HPMo催化剂。然后,在无溶剂条件下,用H _(2)O _(2)评估了各种取代的伯和仲活化苄醇的氧化。在优化的条件下,所有醇都以很高的选择性(≥99%)转化为相应的醛和酮,产率中等至优异(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,这可能归因于GrO纳米片的存在。纳米复合催化剂易于通过常规磁体从反应混合物中回收,并重复使用至少四次,而没有任何结构和催化活性的明显变化。

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