催化剂制备方法对用于腈加氢制饱和胺的负载型Ni催化剂性能的影响

doi:10.1016/S1872-2067(18)63179-1

催化学报 ›› 2019, Vol. 40 ›› Issue (11): 1693-1703.DOI: 10.1016/S1872-2067(18)63179-1

催化剂制备方法对用于腈加氢制饱和胺的负载型Ni催化剂性能的影响

D. J. Segobia, A. F. Trasarti, C. R. Apesteguía

Catalysis Science and Engineering Research Group (GICIC), INCAPE, UNL-CONICET, CCT Conicet-Paraje El Pozo, Santa Fe, 阿根廷

收稿日期:2018-10-03 修回日期:2018-10-12 出版日期:2019-11-18 发布日期:2019-09-06
通讯作者: C. R. Apesteguía

Effect of the catalyst preparation method on the performance of Ni-supported catalysts for the synthesis of saturated amines from nitrile hydrogenation

D. J. Segobia, A. F. Trasarti, C. R. Apesteguía

Catalysis Science and Engineering Research Group (GICIC), INCAPE, UNL-CONICET, CCT Conicet-Paraje El Pozo, (3000) Santa Fe, Argentina

Received:2018-10-03 Revised:2018-10-12 Online:2019-11-18 Published:2019-09-06
Contact: C. R. Apesteguía

摘要/Abstract

摘要： 采用浸渍法（Ni/SiO₂-I）或氨法（Ni/SiO₂-A）制备了硅胶负载的Ni催化剂，考察了它们和Ni/SiO₂-Al₂O₃-I样品催化丁腈液相加氢制备饱和胺反应性能.Ni/SiO₂-I是非酸性催化剂，含有大的Ni⁰颗粒，与载体相互作用较弱；而Ni/SiO₂-A中含有低还原度的Ni-层状硅酸盐，存在Ni²⁺物种，因而是酸性催化剂.在Ni/SiO₂-I催化剂上反应产物基本上是丁胺（80%），副产物仅为二丁胺.相反，以Ni/SiO₂-A为催化剂时，得到二丁胺（49%）和三丁胺（45%）的混合物，而丁胺的生成活性几乎完全得到抑制.对于Ni/SiO₂-A催化剂，丁胺强吸附在邻近Ni⁰原子的表面酸性位上，在反应过程中不能扩散到液相中，从而促进了吸附的丁基亚胺/丁胺物种之间缩合生成更高级的胺类，因此造成选择性生成伯胺和仲胺.

关键词: 腈加氢, 饱和胺, 负载型Ni催化剂, 催化剂制备, 镍-层状硅酸盐类

Abstract: The liquid-phase hydrogenation of butyronitrile to saturated amines was studied on sili-ca-supported Ni catalysts prepared by either incipient-wetness impregnation (Ni/SiO₂-I) or ammonia (Ni/SiO₂-A) methods. A Ni/SiO₂-Al₂O₃-I sample was also used. Ni/SiO₂-I was a non-acidic catalyst containing large Ni⁰ particles of low interaction with the support, while Ni/SiO₂-A was an acidic catalyst due to the presence of Ni²⁺ species in Ni phyllosilicates of low reducibility. Ni/SiO₂-I formed essentially butylamine (80%), and dibutylamine as the only byproduct. In contrast, Ni/SiO₂-A yielded a mixture of dibutylamine (49%) and tributylamine (45%), being the formation of butylamine almost completely suppressed. The selective formation of secondary and tertiary amines on Ni/SiO₂-A was explained by considering that butylamine is not release to the liquid phase during the reaction because it is strongly adsorbed on surface acid sites contiguous to Ni⁰ atoms, thereby favoring the butylimine/butylamine condensation to higher amines between adsorbed species.

Key words: Nitrile hydrogenation, Saturated amines, Ni-supported catalysts, Ni-phyllosilicates, Catalyst preparation

D. J. Segobia, A. F. Trasarti, C. R. Apesteguía. 催化剂制备方法对用于腈加氢制饱和胺的负载型Ni催化剂性能的影响[J]. 催化学报, 2019, 40(11): 1693-1703.

D. J. Segobia, A. F. Trasarti, C. R. Apesteguía. Effect of the catalyst preparation method on the performance of Ni-supported catalysts for the synthesis of saturated amines from nitrile hydrogenation[J]. Chinese Journal of Catalysis, 2019, 40(11): 1693-1703.

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催化剂制备方法对用于腈加氢制饱和胺的负载型Ni催化剂性能的影响

Effect of the catalyst preparation method on the performance of Ni-supported catalysts for the synthesis of saturated amines from nitrile hydrogenation

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