高等学校化学学报 ›› 2019, Vol. 40 ›› Issue (8): 1686-1696.doi: 10.7503/cjcu20190068

• 物理化学 • 上一篇    下一篇

以NiAl-NO3-LDH为前驱体制备Ni-Al2O3催化剂及其催化乙酰丙酸加氢性能

张因, 郭健健, 王杰, 李海涛, 赵永祥   

  1. 山西大学化学化工学院, 精细化学品教育部工程研究中心, 太原 030006
  • 收稿日期:2019-01-23 修回日期:2019-07-23 出版日期:2019-08-10 发布日期:2019-08-02
  • 通讯作者: 赵永祥,男,博士,教授,主要从事多相催化方面的研究.E-mail:yxzhao@sxu.edu.cn E-mail:yxzhao@sxu.edu.cn
  • 基金资助:
    国家自然科学基金(批准号:21303097)和山西省国际科技合作项目(批准号:201803D421074)资助.

Preparation of Ni-Al2O3 Catalysts Derived from Hydrotalcite and Its Catalytic Performance for Hydrogenation of Levulinic Acid

ZHANG Yin, GUO Jianjian, WANG Jie, LI Haitao, ZHAO Yongxiang   

  1. Engineering Research Center of Ministry of Education for Fine Chemicals, School of Chemistry and Chemical Engineering, Shanxi University, Taiyuan 030006, China
  • Received:2019-01-23 Revised:2019-07-23 Online:2019-08-10 Published:2019-08-02
  • Supported by:
    Supported by the National Natural Science Foundation of China(No.21303097) and the Shanxi International Science and Technology Cooperation Project, China(No.201803D421074).

摘要: 以NO3-插层类水滑石(NiAl-NO3-LDH)为前驱体制备了一系列不同Ni/Al摩尔比的Ni-Al2O3催化剂,考察了其催化乙酰丙酸液相加氢性能.表征结果表明,随着Ni/Al摩尔比的增加,类水滑石层板结构中存在的游离态γ-AlOOH物种逐步演变为游离的Ni(OH)2物种,制备的催化剂中金属-载体相互作用逐渐减弱,Ni物种分散度逐渐降低,表面酸性中心数量先增多后减少;当Ni/Al摩尔比为3时,所制备的催化剂表面具有最丰富的酸性中心和加氢中心.在酸性中心和加氢中心的协同作用下,该催化剂表现出优异的催化乙酰丙酸加氢合成γ-戊内酯性能及良好的使用稳定性.在160℃,4 MPa氢气条件下反应5 h时,γ-戊内酯的收率最高可达92.7%.

关键词: 乙酰丙酸, Ni-Al2O3催化剂, γ-戊内酯, 催化加氢

Abstract: A series of Ni-Al2O3 catalysts with different Ni/Al molar ratios was prepared using NiAl-NO3-LDH as precursors and characterized by means of N2-physical adsorption, ICP-OES, TG/DTG, XRD, XPS, H2-TPR/TPD and NH3-TPD techniques. The catalytic performance of these catalysts for liquid phase hydrogenation of levulinic acid was valuated. The results demonstrated that with the increasing of Ni/Al molar ratio, isolated γ-AlOOH species evolved dissociative Ni(OH)2 which existed in the hydrotalcite-like laminate structure, the interaction between metal-support in catalyst become weaker, the dispersion of Ni species decreased, surface acidic sites increased first and then decreased. When Ni/Al molar ratio is 3, the catalyst had the most abundant acidic and hydrogenation sites and exhibited the high performance for the hydrogenation of levulinic acid to γ-valerolactone. 92.7% yield of γ-valerolactone was obtained under the condition of 160℃, 4 MPa H2 pressure.

Key words: Levulinic acid, Ni-Al2O3 catalyst, γ-Valerolactone, Catalytic hydrogeation

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