化工学报2017,Vol.68Issue(11):4161-4168,8.DOI:10.11949/j.issn.0438-1157.20170546
核壳结构镍基纳米催化剂的制备及其在肉桂醛加氢反应中的性能
Preparation of nickel based core-shell catalysts and their catalytic hydrogenation of cinnamaldehyde
摘要
Abstract
Two novel magnetic mesoporous core-shell nanocomposites Ni@mSiO2 and Ni-N2H4@mSiO2 were prepared by a surfactant-templating method. Nickel nanoparticles were first obtained from nickel nitrate or nickel chloride by thermodecomposition and hydrazine hydrate reduction, then covered by a mesoporous shell, and finally by sinteration and hydrogen reduction. As a comparison, Ni/mSiO2 carrier supporting catalyst was prepared by the traditional coprecipitation method. The core-shell nanocomposite of nickel nanoparticle core and mesoporous silica shell was characterized by transmission electron microscopy, X-ray diffraction and nitrogen adsorption-desorption. Temperature programmed H2reduction indicated that NiO in these catalysts were mainly present in bulk phase and some small NiO particles in Ni-N2H4@mSiO2 were easily reduced. H2-chemsorption results demonstrated that Ni/mSiO2 had more active sites but lower TOF value compared to core-shell Ni@mSiO2 and Ni-N2H4@mSiO2 catalysts. Both Ni@mSiO2 and Ni-N2H4@mSiO2 showed higher activity and better selectivity than Ni/mSiO2in selective hydrogenation of cinnamyl aldehyde to hydrocinnamaldehyde, with over 90% yield of hydrocinnamaldehyde. Due to high magnetic saturation value of Ni-N2H4@mSiO2, it can be easily recycled for reuse by an external magnetic field. Notably, Ni-N2H4@mSiO2 showed better stability in hydrogenation.关键词
催化剂/纳米粒子/加氢/核壳结构/构效关系Key words
catalyst/nano particle/hydrogenation/core-shell structure/structure-function relationship分类
化学化工引用本文复制引用
牛立博,刘辰,马苑媛,张慧玲,白国义..核壳结构镍基纳米催化剂的制备及其在肉桂醛加氢反应中的性能[J].化工学报,2017,68(11):4161-4168,8.基金项目
国家自然科学基金项目(21376060,21676068) (21376060,21676068)
河北省自然科学基金项目(B2016201167) (B2016201167)
河北省高等学校科学技术研究项目(QN2015037). supported by the National Natural Science Foundation of China (21376060, 21676068), the Natural Science Foundation of Hebei Province (B2016201167) and the Science and Technology Research Project of Hebei Higher Education (QN2015037). (QN2015037)