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

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 PdCu MAs exhibit a high ethylamine selectivity of 95.38%, yield rate of 1151.07 mmol h g 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 in membrane electrode assembly. Density functional theory calculation reveals that the unique 3D structure and lattice strain of the PdCu MAs synergistically enhance acetonitrile adsorption, and lower the activation barriers of CHCHNH to CHCHNH and CHCHNH to CHCHNH, 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.