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Multi-walled Carbon Nanotubes Supported Nickel Nanoparticles Doped with Magnesia and Copper for Adiponitrile Hydrogenation with High Activity and Chemoselectivity under Mild Conditions
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2018-04-07
Yang Lv, Jun Li, Sheng Feng, Pingle Liu, Fang Hao, Wei Xiong, He'an Luo

Multi-walled carbon nanotubes supported nickel nanoparticles doped with magnesia and copper catalysts were prepared by incipient wetness impregnation method and used in adiponitrile (ADN) hydrogenation to 6-aminohexanenitrile (ACN) and 1,6-hexanediamine (HMDA). The prepared catalysts were characterized by X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), transmission electron microscopy (TEM), high resolution transmission electron microscopy (HRTEM), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), scanning electron microscopy (SEM) and energy dispersive X-ray (EDX), temperature-programmed hydrogen reduction (H2-TPR), H2 chemisorption, temperature-programmed ammonia desorption (NH3-TPD), temperature-programmed carbon dioxide desorption (CO2-TPD) and N2 adsorption-desorption. The results showed that the introduction of magnesia could lead to form NiO-MgO eutectic so as to restrain the reduction of nickel oxide, and it might increase the alkaline site which is conducive to the formation of primary amines in ADN hydrogenation so as to increase the selectivity to ACN and HMDA. Moreover, the formation of NiO-MgO eutectic can also inhibit the sintering of nickel in a certain extent, hence promote the nickel dispersion. And it was revealed that doping of copper can highly promote the catalytic activity by attributing to the strong synergetic effect between copper and nickel which can lead to better dispersion of nickel nanoparticles, larger metallic surface area, lower reduction activation energy of nickel oxide precursor and higher ratio of Ni0+ on the surface of the support. Multi-walled carbon nanotubes supported nickel nanoparticles doped with copper and magnesia presents the best catalytic performance of 96.27% conversion of ADN and 91.22% selectivity to ACN and HMDA under 2 MPa and lower temperature of 328 K.



中文翻译:

多壁碳纳米管负载镁和铜掺杂的镍纳米粒子在温和条件下的高活性和化学选择性对己二腈的氢化反应

采用湿润浸渍法制备了多壁碳纳米管负载的氧化镁和铜催化剂掺杂的镍纳米粒子,并用于己二腈(ADN)加氢成6-氨基己腈(ACN)和1,6-己二胺(HMDA)。通过X射线光电子能谱(XPS),X射线衍射(XRD),透射电子显微镜(TEM),高分辨率透射电子显微镜(HRTEM),高角度环形暗场扫描透射电子显微镜对制备的催化剂进行了表征。 (HAADF-STEM),扫描电子显微镜(SEM)和能量色散X射线(EDX),程序升温的氢气还原(H 2 -TPR),H 2化学吸附,程序升温的氨解吸(NH 3-TPD),程序升温的二氧化碳脱附(CO 2 -TPD)和N 2吸附-解吸。结果表明,氧化镁的引入可以形成NiO-MgO共晶,从而抑制氧化镍的还原,并可能增加碱位,有利于ADN加氢中伯胺的形成,从而增加了氧化镍的生成。对ACN和HMDA的选择性。而且,NiO-MgO共晶的形成还可以在一定程度上抑制镍的烧结,从而促进镍的分散。揭示了铜的掺杂可以归因于铜和镍之间的强协同作用,从而可以大大提高镍纳米颗粒的分散性,更大的金属表面积,更低的氧化镍前体还原活化能和更高的催化活性,从而大大提高了催化活性。 Ni 0+的比例在支撑物的表面上。在2 MPa和328 K的较低温度下,多壁碳纳米管负载的铜和氧化镁掺杂的镍纳米粒子表现出最佳的催化性能,ADN转化率为96.27%,对ACN和HMDA的选择性为91.22%。

更新日期:2018-04-07
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