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Synthesis of highly thermostable copper-nickel nanoparticles confined in the channels of ordered mesoporous SBA-15 silica

机译:限制在有序介孔SBA-15二氧化硅通道中的高耐热铜镍纳米粒子的合成

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摘要

CuNi nanoparticles were effectively confined in the mesopores of SBA-15 silica by a simple incipient wetness impregnation method. After impregnation, the samples were dried at room temperature, which is considered as the key preparation step to obtain high and stable dispersions of the supported CuNi nanoparticles, irrespective of the thermal conditions during the calcination and reduction steps. The catalysts were systematically characterized by powder X-ray diffraction at low and high angles, transmission electron microscopy and nitrogen physisorption, hydrogen temperature-programmed reduction, in situ XRD after temperature-programmed reduction, hydrogen chemisorption as well as by catalytic tests for the hydrogenation of cinnamaldehyde in liquid phase. Characterization revealed a strong interaction between Cu and Ni, resulting in improved reducibility as compared to either Cu or Ni monometallic materials. Moreover, the complete interdiffusion of Cu and Ni atoms to form continuous solid alloy solutions is prevented due to the stabilization of Ni by 1 : 1 nickel phyllosilicate. As a result, the bimetallic CuNi/SBA-15 materials present two distinct metallic phases, one rich in copper and another rich in nickel. At the calcination temperature of 500 °C, the materials displayed the highest chemisorption capacity and highest catalytic activity, as well. Nevertheless, the chemoselectivity of supported CuNi/SBA-15 to cinnamyl alcohol or hydrocinnamaldehyde does not depend on the calcination conditions.
机译:通过简单的初期湿润浸渍方法,将CuNi纳米颗粒有效地限制在SBA-15二氧化硅的中孔中。浸渍后,将样品在室温下干燥,这被认为是关键的制备步骤,以获得高且稳定的负载型CuNi纳米粒子分散体,而与煅烧和还原步骤中的热条件无关。通过低角度和高角度粉末X射线衍射,透射电子显微镜和氮气物理吸附,氢气程序升温还原,程序升温还原后原位XRD,氢气化学吸附以及加氢的催化试验对催化剂进行了系统表征液相中的肉桂醛。表征表明,与铜或镍单金属材料相比,铜和镍之间存在强相互作用,从而导致还原性提高。此外,由于Ni通过1:1的层状硅酸镍稳定化,阻止了Cu和Ni原子的完全相互扩散以形成连续的固态合金溶液。结果,双金属CuNi / SBA-15材料呈现两种截然不同的金属相,一种富含铜,另一种富含镍。在煅烧温度为500°C时,该材料也显示出最高的化学吸附能力和最高的催化活性。然而,负载的CuNi / SBA-15对肉桂醇或氢肉桂醛的化学选择性不取决于煅烧条件。

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