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

doi:10.1016/j.cjche.2021.05.042

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

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

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

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/Abstract

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

Hualiang An, Rui Wang, Wenhao Wang, Daolai Sun, Xinqiang Zhao, Yanji Wang. A core–shell Ni/SiO₂@TiO₂ catalyst for highly selective one-step synthesis of 2-propylheptanol from n-pentanal[J]. 中国化学工程学报, 2022, 46(6): 104-112.

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

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

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