A novel defective PdMo bimetallene with atomic-scale cavities for highly efficient chemicals-assisted hydrogen production

Introducing defects into Pd-based metallene has been shown to significantly enhance its electrocatalytic performance. In this study, we embedded a new type of atomic-scale cavities into the basal plane of PdMo bimetallene (c-PdMo) through precise etching. These cavities introduced tensile strain and increased the generalized coordination number (CN̅), resulting in superior performance in formate oxidation reaction (FOR) and methanol oxidation reaction (MOR), with mass activities of 5.01 mAμgNM−1 and 5.38 mAμgNM−1, respectively. Notably, a two-electrode system comprising commercial Pt/C and c-PdMo coated on carbon paper achieved cell voltages of only 0.517 V and 0.362 V at 10 mA cm−2 for FOR and MOR, respectively. Additionally, density functional theory calculations revealed that the deliberate lattice tensile strain and enhanced coordination numbers reduced the D-band center of defective PdMo, which improved OH adsorption and reduced CO adsorption, thus optimizing FOR and MOR catalysis on the surface of c-PdMo bimetallene.