Modifying the atomic and electronic structure of platinum-based alloy to enhance its activity and anti-CO poisoning ability is a vital issue in hydrogen oxidation reaction (HOR). However, the role of foreign modifier metal and the underlying ligand effect is not fully understood. Here, we propose that the ligand effect of single-atom Cu can dynamically modulate the d-band center of Pt-based alloy for boosting HOR performance. By in situ X-ray absorption spectroscopy, our research has identified that the potential-driven structural rearrangement into high-coordination Cu-Pt/Pd intensifies the ligand effect in Pt-Cu-Pd, leading to enhanced HOR performance. Thereby, modulating the d-band structure leads to near-optimal hydrogen/hydroxyl binding energies and reduced CO adsorption energies for promoting the HOR kinetics and the CO-tolerant capability. Accordingly, PtPdCu/C exhibits excellent CO tolerance even at 1,000 ppm impurity.
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