Manipulating d-band Center by Interface-Induced Dislocation in Pt@PtCu Nanowires Boosting Oxygen Reduction

Abstract

Engineering the electronic configuration and intermediates adsorption behaviors of Platinum-based catalysts is crucial for improving oxygen reduction reaction (ORR) kinetics at the cathode in proton exchange membrane fuel cells (PEMFCs), yet it remains an enormous challenge. Herein, an interface-induced dislocation tactic through Pt/PtCu heterogeneous formation in Pt@PtCu nanowires composites (Pt@PtCu NWs) for efficient ORR is reported. Theoretical studies have proven that dislocation driven by a hybrid interface could alter electron redistribution and downshift the d-band of Pt, thus facilitating the desorption of oxygen-containing species and achieving outstanding ORR performance. Specifically, the as-prepared Pt@PtCu NWs deliver exceptional ORR properties with a half-wave of 0.940 V. Moreover, the mass activity (MA) of Pt@PtCu NWs reaches 1.17 A mgPt−1 at 0.9 V, which is 4.18 and 10.64 times higher than that of Pt NWs (0.27 A mgPt−1) and commercial Pt/C (0.11 A mgPt−1). Most importantly, Pt@PtCu NWs also prove remarkable structural stability with only a 14.5% decrease in MA compared to a 58.9% decrease for Pt/C after the durability test. Overall, this strategy of d-band center tuning induced by hybrid-interface-driven dislocation provides a promising avenue for designing high-efficiency electrocatalysts.