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Minimizing the Size of Palladium Nanoparticles Immobilized within the Channels of Ionic Liquid-Derived Magnetically Separable Heteroatom-Doped Mesoporous Carbon for Aerobic Oxidation of Alcohols
ACS Applied Nano Materials ( IF 5.9 ) Pub Date : 2020-10-30 , DOI: 10.1021/acsanm.0c01780
Babak Karimi 1, 2 , Fariborz Mansouri 1 , Hojatollah Vali 3
Affiliation  

An efficient and well-designed nanocasting procedure has been developed for the synthesis of a series of nitrogen and sulfur codoped magnetically separable ordered mesoporous carbons using an imidazolium-based ionic liquid as the carbon source, guanine as the nitrogen source, FeCl3 as the iron source, and SBA-15 as the hard template. The role of different percentage of the guanine as the nitrogen source on the uniformity of the mesochannels and physicochemical properties of the prepared materials was fully investigated using various techniques including N2 sorption analysis, TEM, FESEM, XRD, AAS, XPS, Raman spectroscopy, CHN, VSM, elemental mapping, and FT-IR. It was observed that large amounts of small and monodispersed iron oxide nanoparticles could be embedded within the carbon rods without any channel blocking, a considerable loss of surface area, and aggregation of nanoparticles. It was also found that both the nitrogen content and surface area of the material have a crucial synergistic effect on the production of small and monodispersed Pd nanoparticles within the carbon pores. The smaller size and more uniform distribution of the Pd nanoparticles produced in the Pd@Fe-GIOMC-40 (in which 40 wt % guanine was employed) resulted in improved catalytic activity in the aerobic oxidation of benzyl alcohol compared to other samples. This catalyst demonstrated outstanding activity in direct and selective oxidation of primary alcohols into the corresponding carboxylic acids under aqueous conditions using very low amounts of catalyst. Importantly, it was found that its activity was completely switchable since it provided a useful procedure for the oxidation of primary alcohols into aldehydes under controlled reaction conditions (in toluene as a solvent instead of water). The catalyst could be simply separated from the reaction mixture using an external magnet and reused in both aqueous and organic reaction media for the next six successive runs with no considerable loss of activity.

中文翻译:

最小化固定在离子液体衍生的磁可分离杂原子掺杂的介孔碳通道中的钯纳米颗粒的尺寸,以用于乙醇的好氧氧化

已经开发了一种有效且设计良好的纳米铸造程序,用于使用咪唑基离子液体作为碳源,鸟嘌呤作为氮源,FeCl 3作为铁来合成一系列氮和硫共掺杂的磁可分离有序介孔碳。源,并将SBA-15作为硬模板。使用包括N 2在内的各种技术,充分研究了不同百分比的鸟嘌呤作为氮源对介孔通道的均匀性和所制备材料的理化性质的作用。吸附分析,TEM,FESEM,XRD,AAS,XPS,拉曼光谱,CHN,VSM,元素图谱和FT-IR。观察到,大量的小且单分散的氧化铁纳米粒子可以嵌入碳棒中,而没有任何通道阻塞,相当大的表面积损失和纳米粒子聚集。还发现,材料的氮含量和表面积都对碳孔内小的单分散的Pd纳米颗粒的生产具有至关重要的协同作用。与其他样品相比,Pd @ Fe-GIOMC-40(其中使用40 wt%鸟嘌呤)中产生的Pd纳米粒子的尺寸更小且分布更均匀,从而改善了苯甲醇的好氧氧化催化活性。该催化剂显示了在水性条件下使用非常少量的催化剂将伯醇直接和选择性氧化为相应羧酸的出色活性。重要的是,发现它的活性是完全可切换的,因为它提供了在受控反应条件下(在甲苯中代替水而不是在水中)将伯醇氧化成醛的有用方法。可以使用外部磁体将催化剂简单地从反应混合物中分离出来,然后再用于水性和有机反应介质中,以进行接下来的六次连续运行,而不会损失活性。发现它的活性是完全可切换的,因为它提供了在受控反应条件下(以甲苯代替水代替溶剂)将伯醇氧化为醛的有用方法。可以使用外部磁体将催化剂简单地从反应混合物中分离出来,然后再用于水性和有机反应介质中,以进行接下来的六次连续运行,而不会损失活性。发现它的活性是完全可切换的,因为它提供了在受控反应条件下(以甲苯代替水代替溶剂)将伯醇氧化为醛的有用方法。可以使用外部磁体将催化剂简单地从反应混合物中分离出来,然后再用于水性和有机反应介质中,以进行接下来的六次连续运行,而不会损失活性。
更新日期:2020-10-30
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