Insight into the mechanism of acetonitrile hydrogenation in liquid phase on Pt/Al2O3 by ATR-FTIR

被引:24
作者
Aguirre, Alejo [1 ]
Collins, Sebastian E. [1 ]
机构
[1] Univ Nacl Litoral, CONICET, Inst Desarrollo Tecnol Ind Quim INTEC, Guemes 3450,S3000GLN, Santa Fe, Argentina
关键词
Nitrile hydrogenation; Attenuated total reflection; Amines; Platinum; IN-SITU; CATALYTIC-HYDROGENATION; INFRARED-SPECTRA; H/D EXCHANGE; ADSORPTION; NITRILES; AMINES; ETHYLAMINE; ELECTRODES; AMMONIA;
D O I
10.1016/j.cattod.2019.04.027
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
The mechanism of the acetonitrile hydrogenation to amines over a platinum/alumina catalyst was investigated by in situ infrared spectroscopy. The reaction was studied under realistic conditions -liquid phase using toluene as solvent-using a flow-through cell-microreactor in Attenuated Total Reflection (ATR) mode. Acetonitrile linearly chemisorbed on platinum sites is stepwise hydrogenated to form an imine surface intermediate (CH3CH = NH), which in turn is hydrogenated to ethylamine. Using deuterium, the sequential formation of C-D and N-D bonds was observed. Then, imine intermediate can condense producing diethylamine and triethylamine, giving ammonia as a by-product. The temporal evolution of the IR signals was modeled using a proposed microkinetic mechanism and intrinsic kinetic constants were obtained under chemical control.
引用
收藏
页码:22 / 32
页数:11
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