Low-Coordinated Pd–Pb Sites in Porous Pd3Pb Metallene Aerogels Promote Polyalcohol Electrochemical Oxidation

Abstract

Low-coordinated sites can effectively activate adsorbants and promote electrochemical reactions with slow kinetics and multielectron transfer processes, but achieving high exposure rates of low-coordinated sites on the electrocatalyst surface remains challenging. Herein, we first present the synthesis of the porous Pd₃Pb metallene aerogels (MAs) with low-coordinated Pd–Pb sites through dynamic reconfiguration strategy for alcohol oxidation reaction (AOR). The porous Pd₃Pb MAs possess high mass activity (1.63 A mg_Pd^–1), specific activity (6.28 mA cm^–2), and antipoisoning property in ethylene glycol oxidation reaction (EGOR), superior to other prepared catalysts. The same trend was observed in the ethanol oxidation reaction and glycerol oxidation reaction. Mechanism studies show that porous Pd₃Pb MAs with low-coordinated Pd–Pb sites could provide more unsaturated sites for adsorption and activation of ethylene glycol, as well as lowering the reaction energy barriers of CH₂OHCHO*, CH₂OHCOO*, and COOCOO*. This work explored a novel idea for the design Pd-based catalysts in antipoisoned AOR.