SCI和EI收录∣中国化工学会会刊

中国化学工程学报 ›› 2022, Vol. 46 ›› Issue (6): 104-112.DOI: 10.1016/j.cjche.2021.05.042

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A core–shell Ni/SiO2@TiO2 catalyst for highly selective one-step synthesis of 2-propylheptanol from n-pentanal

Hualiang An, Rui Wang, Wenhao Wang, Daolai Sun, Xinqiang Zhao, Yanji Wang   

  1. Hebei Provincial Key Laboratory of Green Chemical Technology and Efficient Energy Saving, Tianjin Key Laboratory of Chemical Process Safety, School of Chemical Engineering and Technology, Hebei University of Technology, Tianjin 300130, China
  • 收稿日期:2021-02-24 修回日期:2021-04-28 出版日期:2022-06-28 发布日期:2022-07-20
  • 通讯作者: Xinqiang Zhao,E-mail:zhaoxq@hebut.edu.cn
  • 基金资助:
    This work was financially supported by the National Natural Science Foundation of China (21978066, 21506046), Natural Science Foundation of Hebei Province (B2020202048, B2018202220), and Natural Science Foundation of Tianjin City (18JCYBJC42600). The authors are gratefully appreciative of their contributions.

A core–shell Ni/SiO2@TiO2 catalyst for highly selective one-step synthesis of 2-propylheptanol from n-pentanal

Hualiang An, Rui Wang, Wenhao Wang, Daolai Sun, Xinqiang Zhao, Yanji Wang   

  1. Hebei Provincial Key Laboratory of Green Chemical Technology and Efficient Energy Saving, Tianjin Key Laboratory of Chemical Process Safety, School of Chemical Engineering and Technology, Hebei University of Technology, Tianjin 300130, China
  • Received:2021-02-24 Revised:2021-04-28 Online:2022-06-28 Published:2022-07-20
  • Contact: Xinqiang Zhao,E-mail:zhaoxq@hebut.edu.cn
  • Supported by:
    This work was financially supported by the National Natural Science Foundation of China (21978066, 21506046), Natural Science Foundation of Hebei Province (B2020202048, B2018202220), and Natural Science Foundation of Tianjin City (18JCYBJC42600). The authors are gratefully appreciative of their contributions.

摘要: One-step synthesis of 2-propylheptanol (2-PH) from n-pentanal via a reaction integration of n-pentanal self-condensation and successive hydrogenation is of great significance for it can simplify process flow and reduce energy consumption. The key to promotion of 2-PH selectivity is to enhance the competitiveness of n-pentanal self-condensation with respect to its direct hydrogenation. For this purpose, a core–shell structured Ni/SiO2@TiO2 catalyst was designed and prepared. With the precise architecture of this core–shell structured catalyst, n-pentanal can be firstly in contact with TiO2 to 2-propyl-2-heptenal (2-PHEA) while the direct hydrogenation to n-pentanol can be effectively inhibited, and then 2-PHEA diffuses into the core of Ni/SiO2 and is hydrogenated to 2-PH. The spatial threshold of the core–shell catalyst significantly enhanced its catalytic performance; a 2-PH selectivity of 77.9% was reached with a 100% n-pentanal conversion. The 2-PH selectivity is much higher than that obtained by employing Ni/TiO2 catalyst. Furthermore, the reaction kinetics of one-step synthesis of 2-PH from n-pentanal catalyzed by Ni/SiO2@TiO2 was studied and its kinetic model was established which is useful for reactor design and scale-up.

关键词: Reaction integration, n-Pentanal, 2-Propylheptanol, Core-shell structure, Reaction kinetics

Abstract: One-step synthesis of 2-propylheptanol (2-PH) from n-pentanal via a reaction integration of n-pentanal self-condensation and successive hydrogenation is of great significance for it can simplify process flow and reduce energy consumption. The key to promotion of 2-PH selectivity is to enhance the competitiveness of n-pentanal self-condensation with respect to its direct hydrogenation. For this purpose, a core–shell structured Ni/SiO2@TiO2 catalyst was designed and prepared. With the precise architecture of this core–shell structured catalyst, n-pentanal can be firstly in contact with TiO2 to 2-propyl-2-heptenal (2-PHEA) while the direct hydrogenation to n-pentanol can be effectively inhibited, and then 2-PHEA diffuses into the core of Ni/SiO2 and is hydrogenated to 2-PH. The spatial threshold of the core–shell catalyst significantly enhanced its catalytic performance; a 2-PH selectivity of 77.9% was reached with a 100% n-pentanal conversion. The 2-PH selectivity is much higher than that obtained by employing Ni/TiO2 catalyst. Furthermore, the reaction kinetics of one-step synthesis of 2-PH from n-pentanal catalyzed by Ni/SiO2@TiO2 was studied and its kinetic model was established which is useful for reactor design and scale-up.

Key words: Reaction integration, n-Pentanal, 2-Propylheptanol, Core-shell structure, Reaction kinetics