Pd/Ni(OH) ₂ Derived Catalysts for Selective Electrosynthesis of Ethylamine

Abstract Replacing traditional chemical manufacture with renewable energy‐powered electrochemical routes offers a promising means for decarbonization. An important target compound is ethylamine with important applications as a building block for chemical synthesis and potentially as a green hydrogen carrier. However, to enable operation at economically competitive levels, there is a need to develop more efficient catalysts and reactor systems. Here, we show that catalysts derived from Ni(OH) 2 are selective toward the electrochemical reduction of acetonitrile to ethylamine in a membrane electrode assembly (MEA) system. We further found that selectivity can be further improved via Pd doping, with Pd/Ni(OH) 2 exhibiting a Faradaic efficiency of 96.1% at 80 mA cm −2 . Furthermore, we successfully demonstrated stable performance with Pd/Ni(OH) 2 over a 25 h operating period. Using density functional theory (DFT) calculations, we found that the addition of Pd enhances performance by promoting the adsorption of *CH 3 CN and desorption of *CH 3 CH 2 NH 2 .