Amorphous MoOxwith High Oxophilicity Interfaced with PtMo Alloy Nanoparticles Boosts Anti‐CO Hydrogen Electrocatalysis

Abstract

AbstractAdvancing electrocatalysts for alkaline hydrogen oxidation/evolution reaction (HOR/HER) is essential for anion exchange membrane‐based devices. The state‐of‐the‐art Pt‐based electrocatalysts for alkaline HOR suffer from low intrinsic activities and severe CO poisoning due to the challenge of simultaneously optimizing surface adsorption toward different adsorbates. Herein, this challenge is overcome by tuning an atomic MoOxlayer with high oxophilicity onto PtMo nanoparticles (NPs) with optimized Had, OHad, and COadadsorption for boosting anti‐CO‐poisoning hydrogen‐cycle electrocatalysis in alkaline media. For alkaline HOR, this catalyst exhibits high kinetics and an exchange current density of 3.19 mA µgPt−1at 50 mV versus reversible hydrogen electrode and 0.83 mA cmPt−2, 10.3‐ and 3.8‐fold higher than those of commercial Pt/C, respectively. For alkaline HER, it achieves an unprecedented overpotential of 37 mV at 10 mA cm−2. Experimental and theoretical studies show that the orchestrated electronic and oxophilic regulation of the PtMo/MoOxinterface NPs simultaneously optimizes Hadand OHadadsorption for boosting alkaline hydrogen electrocatalysis, whereas reactive oxygen from the amorphous MoOxatomic layer lowers the CO oxidation reaction barrier, leading to superior anti‐poisoning ability even at 100 ppm CO.