Hao Yufen, Cárdenas-Lizana Fernando, Keane Mark A
Chemical Engineering, School of Engineering and Physical Sciences, Heriot-Watt University, Edinburgh, EH14 4AS Scotland, UK.
Catal Letters. 2017;147(4):803-810. doi: 10.1007/s10562-016-1902-7. Epub 2017 Feb 14.
The catalytic (Pd/AlO and Pd/C; mean Pd size 2.5-3.0 nm from (S)TEM analysis) synthesis of di-butylamine (DBA) and tri-butylamine (TBA) from mono-butylamine (MBA) and DBA, respectively, in continuous gas phase operation is demonstrated. Exclusive production of DBA (from MBA) has been established over both catalysts where 453 ≤ ≤ 523 K (∆E = 79 kJ mol). Greater activity for Pd/C is associated with higher levels of surface acidity (from NH chemisorption/TPD) and spillover hydrogen (from H TPD). Reaction of DBA over both catalysts when configured in series delivered full selectivity to TBA. Our results establish a novel clean alternative route for the continuous production of higher (secondary and tertiary) amines.
本文展示了在连续气相操作中,分别以单丁胺(MBA)和二丁胺(DBA)为原料,通过催化作用(Pd/AlO和Pd/C;经(S)TEM分析,平均钯粒径为2.5 - 3.0纳米)合成二丁胺(DBA)和三丁胺(TBA)的过程。在两种催化剂上均已实现从MBA独家生产DBA,反应温度为453 ≤ ≤ 523 K(∆E = 79 kJ mol)。Pd/C具有更高的活性,这与更高水平的表面酸度(通过NH化学吸附/TPD测定)和溢流氢(通过H TPD测定)有关。当两种催化剂串联配置时,DBA在两种催化剂上的反应对TBA具有完全选择性。我们的研究结果为连续生产高级(仲胺和叔胺)胺建立了一种新型的清洁替代路线。