Heterogeneous Ru-Based Catalysts for One-Pot Synthesis of Primary Amines from Aldehydes and Ammonia
Heterogeneous Ru-Based Catalysts for One-Pot Synthesis of Primary Amines from Aldehydes and Ammonia
复制标题
用于醛和氨一锅法合成伯胺的多相钌基催化剂
DOI：
10.3390/catal5042258
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发表时间：
2015-12-01
期刊：
影响因子：
3.9
通讯作者：
Mu, Xindong
中科院分区：
文献类型：
--
作者：
Dong, Bo;Guo, Xingcui;Mu, Xindong
羰基化合物与NH3和H2-的直接还原胺化是生产伯胺的一种替代路线。寻找高效和选择性的催化剂已经引起了极大的兴趣。研究了钌基催化剂上庚醛与氨的还原胺化反应。产物选择性与钌的载体有关。具有尖晶石结构的氧化铝（-Al_2O_3，-Al_2O_3）负载的Ru催化剂在最佳条件下，在100%庚醛转化率下表现出有利于伯胺的选择性（94%产率）。碱性（MgO、CaO）和相对酸性（Nb_2 O_5、SnO_2、MCM-41、HZSM-5）载体对伯胺显示相对差的选择性（0%-53%产率）。并提出了还原胺化机理。Schiff碱N-[庚烯]庚基-1-胺是关键中间体。Ru/-Al_2 O_3是一种优良的氢解催化剂，可用于N-庚烯庚基-1-胺的胺化和氢解反应。
The direct reductive amination of carbonyl compounds with NH3 and H-2 is an alternative route to produce primary amines in practical production. The search for efficient and selective catalysts has attracted great interest. In the present work, the reductive amination of heptaldehyde with NH3 was investigated over a Ru-based catalyst. The product selectivities were found to be related with the supports of Ru. The alumina with spinel structure (-Al2O3, -Al2O3)-supported Ru catalysts exhibited selectivity favoring primary amines (94% yield) at 100% heptaldehyde conversion under optimal conditions. Purely basic (MgO, CaO) and relative acidic (Nb2O5, SnO2, MCM-41, HZSM-5) supports showed relatively poor selectivity towards primary amines (0%-53% yield). The reductive amination mechanism was also proposed. The Schiff base N-[heptylene]heptyl-1-amine was a key intermediate. Ru/-Al2O3 was shown to be an excellent hydrogenolysis catalyst to selectively produce primary amine by amination and hydrogenolysis of N-[heptylene]heptyl-1-amine.