Multi-walled carbon nanotubes supported nickel nanoparticles doped with magnesia and copper for adiponitrile hydrogenation with high activity and chemoselectivity under mild conditions
Multi-walled carbon nanotubes supported nickel nanoparticles doped with magnesia and copper for adiponitrile hydrogenation with high activity and chemoselectivity under mild conditions
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多壁碳纳米管负载氧化镁和铜掺杂的镍纳米粒子用于己二腈氢化，在温和条件下具有高活性和化学选择性
DOI：
10.1016/j.cej.2018.04.031
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发表时间：
2018-08
影响因子：
15.1
通讯作者：
Hean Luo
中科院分区：
文献类型：
--
作者：
Yang Lv;Jun Li;Sheng Feng;Pingle Liu;Fang Hao;Wei Xiong;Hean Luo
采用等体积浸渍法制备了多壁碳纳米管负载纳米镍、氧化镁和铜掺杂的催化剂，并将其用于己二腈（ADN）加氢合成6-氨基己腈（ACN）和1，6-己二胺（HMDA）。采用X射线光电子能谱（XPS）、X射线衍射（XRD）、透射电子显微镜（TEM）、高分辨透射电子显微镜（HRTEM）、高角度环形暗场扫描透射电子显微镜（HRTEM）等手段对催化剂进行了表征（HAADF-STEM）、扫描电子显微镜（SEM）和能量色散X射线（EDX）、程序升温氢还原（H2-TPR）、H2化学吸附、程序升温氨脱附（NH_3-TPD）、程序升温二氧化碳脱附（CO_2-TPD）和氮气吸附-脱附。结果表明，氧化镁的引入可导致NiO-MgO共晶的形成，从而抑制氧化镍的还原，并可增加ADN加氢反应中有利于伯胺生成的碱性中心，从而提高ACN和HMDA的选择性。此外，NiO-MgO共晶的形成也在一定程度上抑制了镍的烧结，从而促进了镍的分散。结果表明，铜的掺杂可以提高催化剂的活性，这是由于铜和镍之间的协同效应使镍纳米颗粒分散性更好，金属比表面积更大，氧化镍前驱体的还原活化能更低，载体表面的Ni ~（0+）比例更高。在2 MPa和328 K低温下，Cu和MgO掺杂的多壁碳纳米管负载Ni纳米粒子催化剂对ADN的转化率为96.27%，对ACN和HMDA的选择性为91.22%。
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 adsorptiondesorption. 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 nanoparticlesdoped 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.
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影响因子：
5.5
作者：
F. Medina;P. Salagre;J. Sueiras;J. Fierro
通讯作者：
F. Medina;P. Salagre;J. Sueiras;J. Fierro
酸活化海泡石负载镍钾双金属催化剂改进 1,6-己二腈液相加氢催化性能
DOI：
10.1016/j.molcata.2016.10.029
发表时间：
2017
期刊：
Journal of Molecular Catalysis A: Chemical
影响因子：
--
作者：
Fang Hao;Pingle Liu;Shaofeng Xiong;He'an Luo
通讯作者：
He'an Luo
影响因子：
7.3
作者：
M. Serra;P. Salagre;Y. Cesteros;F. Medina;J. Sueiras
通讯作者：
M. Serra;P. Salagre;Y. Cesteros;F. Medina;J. Sueiras
DOI：
10.1039/ft9938903507
发表时间：
1993
期刊：
Journal of the Chemical Society, Faraday Transactions
影响因子：
--
作者：
F. Medina;P. Salagre;J. Sueiras;J. Fierro
通讯作者：
F. Medina;P. Salagre;J. Sueiras;J. Fierro
影响因子：
2.3
作者：
Saito Y;Ishitani H;Ueno M;Kobayashi S
通讯作者：
Kobayashi S