Lattice‐Strained Pd@Pd─Cu Core─Shell Metallene Aerogels for Electrocatalytic Acetonitrile to Ethylamine

Abstract Lattice strain engineering has been widely validated as a pivotal strategy to enhance electrocatalyst performance in reactions. However, its application in designing catalysts for acetonitrile reduction reaction (ARR) remains unexplored, highlighting a promising yet underexplored avenue to tailor both activity and product selectivity. Herein, for the first time, lattice‐strained Pd@Pd─Cu metallene aerogels (MAs) are developed as efficient and stable effective electrocatalysts for ARR. Notably, the optimized Pd 1.75 Cu MAs exhibit a high ethylamine selectivity of 95.38%, yield rate of 1151.07 mmol h −1 g −1 Pd+Cu and Faradaic efficiency of 93.34% at −0.60 V versus reversible hydrogen electrode (RHE) in H cell, while demonstrate excellent stability throughout a 245 h continuous test at 250 mA cm −2 in membrane electrode assembly. Density functional theory calculation reveals that the unique 3D structure and lattice strain of the Pd 1.75 Cu MAs synergistically enhance acetonitrile adsorption, and lower the activation barriers of CH 3 CHNH * to CH 3 CH 2 NH * and CH 3 CH 2 NH 2 * to CH 3 CH 2 NH 2 , thus boosting the ARR performance. This work not only provides a new paradigm for developing novel ARR electrocatalysts, but also expands the potential of other application areas.