Laser Irradiation Induced Electronic Structure Modulation of the Palladium‐Based Nanosheets for Efficient Electrocatalysts

Palladium nanosheets (Pd NSs) are widely used as electrocatalysts due to their high atomic utilization efficiency, and long‐term stability. Here, the electronic structure modulation of the Pd NSs is realized by a femtosecond laser irradiation strategy. Experimental results indicate that laser irradiation induces the variation in the atomic structures and the macrostrain effects in the Pd NSs. The electronic structure of Pd NSs is modulated by laser irradiation through the balancing between Au–Pd charge transfer and the macros‐strain effects. Finite element analysis (FEA) indicates that the lattice of the nanostructures undergoes fast heating and cooling during laser irradiation. The structural evolution mechanism is disclosed by a combined FEA and molecule dynamics (MD) simulation. These results coincide well with the experimental results. The L‐AuPd NSs exhibit excellent mass activity and specific activity of 7.44 A mg‐1 Pd and 18.70 mA cm −2 toward ethanol oxidation reaction (EOR), 4.3 and 4.4 times higher than the commercial Pd/C. The 2500‐cycle accelerated durability (ADT) test confirms the outstanding catalytic stability of the L‐AuPd NSs. Density functional theory (DFT) calculations reveal the catalytic mechanism. This unique strategy provides a new pathway to design the ultrathin nanosheet‐based materials with excellent performance.