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Insight into the mechanism of acetonitrile hydrogenation in liquid phase on Pt/Al2O3 by ATR-FTIR
Catalysis Today ( IF 5.2 ) Pub Date : 2019-04-09 , DOI: 10.1016/j.cattod.2019.04.027
Alejo Aguirre , Sebastián E. Collins

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 CD and ND 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.



中文翻译:

ATR-FTIR对Pt / Al 2 O 3上液相乙腈加氢机理的认识

通过原位红外光谱研究了铂/氧化铝催化剂上乙腈加氢成胺的机理。在现实条件下对反应进行了研究-使用甲苯作为溶剂的液相-使用流通池式微反应器以衰减全反射(ATR)模式进行研究。将线性化学吸附在铂位上的乙腈逐步氢化以形成亚胺表面中间体(CH 3 CH = NH),然后将其氢化成乙胺。使用氘,依次形成C D和N观察到D键。然后,亚胺中间体可以缩合生成二乙胺和三乙胺,从而产生氨副产物。使用提出的微动力学机制对红外信号的时间演变进行建模,并在化学控制下获得内在动力学常数。

更新日期:2019-04-09
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