Building a Microkinetic Model from First Principles for Higher Amine Synthesis on Pd Catalyst

The hydrogenation of nitriles utilizing heterogeneous catalysis is a significant commercial process for the synthesis of primary, secondary, and tertiary amines. Periodic plane-wave density functional theory (DFT) is used to examine the hydrogenation of acetonitrile to primary, secondary, and tertiary amines on palladium catalysts. The quantified minimum energy reaction pathways, including activation barriers, for acetonitrile reaction to higher amines are discussed. The construction of a microkinetic model from first-principles for higher amine synthesis is presented. In addition, the microkinetic model simulations are discussed and compared to palladium-based catalyst experimental results for higher amine synthesis. For the first time, this novel and robust reactor model provides detailed insights into surface species coverage, as a function of process conditions (e.g., feedstock ratio, catalyst type, temperature, and pressure). More broadly, process engineers can leverage this valuable information to guide reaction engineering efforts, including process optimization, reactor design, and catalyst selection.