Dense Nanopore Reconstruction of Hexagonal PdCu Superstructure for Robust Methanol Electrooxidation

The pore-dense surface of Pd-based nanosheets (NSs) with abundant marginal active sites could offer a great opportunity to enhance alcohol electrocatalysis properties. However, most Pd-based NSs with a porous structure were synthesized in two or more steps with surfactant participation, which lacks favorable simplicity. Herein, we developed an advanced solvent-mediated one-step surfactant-free method to engineer a kind of PdCu superstructure by in situ dense surface nanopores reconstruction. The hexagonal superstructures with dense crystalline/amorphous interfaces and abundant edge active sites were assembled by porous nanosheets (PNSs). Benefiting from the crystalline/amorphous heterostructure nanosheets, highly open structure with rich mass and electron transfer tunnels, and pore-dense surface with plentiful defect-rich active sites, the obtained PdCu PNSs exhibited superior methanol oxidation reaction (MOR) specific activity, which was 1.9 times higher than that of nonpore PdCu NSs with smooth edge. In addition, the PdCu PNSs exhibited an optimal d-band center and favorable original structure stability after stability tests. The study not only revealed the relationship between pore-dense heterophase structure and catalytic performance but also provided an instructive strategy for more synthesis on other surfactant-free porous superstructures.