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 Pd_1.75Cu 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_1.75Cu MAs synergistically enhance acetonitrile adsorption, and lower the activation barriers of CH₃CHNH^* to CH₃CH₂NH^* and CH₃CH₂NH₂ ^* to CH₃CH₂NH₂, 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.