高晓霞,王奖,徐爱菊,贾美林.Ni-Co-Al混合氧化物的制备及其丙烷氧化脱氢催化性能[J].分子催化编辑部,2019,33(6):531-541
Ni-Co-Al混合氧化物的制备及其丙烷氧化脱氢催化性能
Preparation of Ni-Co-Al Mixed Oxides and Their Catalytic Performance for Oxidative Dehydrogenation of Propane
投稿时间:2019-10-10  修订日期:2019-11-15
DOI:
中文关键词:  类水滑石  混合金属氧化物      丙烷氧化脱氢
英文关键词:layered double hydroxide  mixed metal oxide  nickel  cobalt  oxidative dehydrogenation of propane
基金项目:内蒙古自治区水环境安全协同创新培育中心项目(XTCX003);内蒙古自然科学基金(2019MS02016);内蒙古师范大学研究生科研创新基金资助项目(CXJJS18084)
作者单位E-mail
高晓霞 内蒙古师范大学 化学与环境科学学院, 内蒙古自治区绿色催化重点实验室, 内蒙古 呼和浩特 010022  
王奖 内蒙古师范大学 化学与环境科学学院, 内蒙古自治区绿色催化重点实验室, 内蒙古 呼和浩特 010022 wangjfree@163.com 
徐爱菊 内蒙古师范大学 化学与环境科学学院, 内蒙古自治区绿色催化重点实验室, 内蒙古 呼和浩特 010022 xuaj@imnu.edu.cn 
贾美林 内蒙古师范大学 化学与环境科学学院, 内蒙古自治区绿色催化重点实验室, 内蒙古 呼和浩特 010022  
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中文摘要:
      采用恒定pH共沉淀法制备不同Ni/Co摩尔比的3(NixCo1-x)-Al类水滑石前驱体,600℃焙烧得3(NixCo1-x)Al混合氧化物(MMO)催化剂(x=1,0.95,0.90,0.75,0.50,0.25,0),通过电感耦合等离子体发射光谱、N2物理吸附-脱附、X射线衍射和透射电子显微镜表征其组成、表面织构、晶相和微观形貌,考察Ni/Co摩尔比对其丙烷氧化脱氢制丙烯催化性能的影响.结果表明,3(Ni0.90Co0.10)Al MMO催化剂催化性能最佳:丙烯选择性随反应温度升高未发生明显降低,反应温度500℃时丙烷转化率31%、丙烯选择性48%,丙烯收率15%,且催化剂寿命良好.通过X射线光电子能谱、H2程序升温还原和原位电导测试研究发现,掺杂少量Co后催化剂表面Ni(II)与Co(II/III)间存在电子交互作用,表面类NiO相分散性提高,晶格氧物种增多,催化剂具有优良的氧化还原可逆性.
英文摘要:
      A series of 3(NixCo1-x)-Al layered double hydroxide (LDH) precursors with different Ni/Co molar ratios were prepared by a constant pH coprecipitation method. The 3(NixCo1-x)Al mixed oxide (MMO) catalysts (x=1, 0.95, 0.90, 0.75, 0.50, 0.25, 0) were obtained after calcination of the LDH precursors at 600℃. The composition, surface texture, crystal phase and micromorphology of the catalysts were characterized by Inductively Coupled Plasma Emission Spectroscopy (ICP-MS), N2 Physical Adsorption-desorption, X-ray Diffraction (XRD) and Transmission Electron Microscope (TEM). And the effects of Ni/Co molar ratios on their catalytic performance for oxidative dehydrogenation of propane (ODHP) to propylene were investigated. The results showed that 3(Ni0.90-Co0.10)Al MMO catalyst had the best catalytic performance:The propylene selectivity was not decreased obviously with the increase of reaction temperature; the propane conversion was 31%, the propylene selectivity was 48% and the propylene yield was 15% at 500℃; furthermore the stability of the catalyst was excellent. It was considered that there was an electronic interaction between the surface Ni(II) and Co(II/III), the dispersion of the surface NiO-like phase was improved and the surface lattice oxygen species were increased after a small amount of Co doping, then the catalyst showed an excellent reversibility of oxidation-reduction, through the study of X-ray Photoelectron Spectroscopy (XPS), H2 Temperature Programmed Reduction (H2-TPR) and In-situ conductivity measurements.
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