ACS Mater. Lett. - Low-Coordinated Pd-Pb Sites in Porous Pd3Pb Metallene Aerogels Promote Polyalcohol Electrochemical Oxidation
Hui Fu, Zhen Huang, Ting Zhu*, Liheng Guan, Chih-Wen Pao, Wei-Hsiang Huang*, Nan Zhang,* Tianxi Liu*
ACS Mater. Lett. 2024, DOI:10.1021/acsmaterialslett.4c01573
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 mgPd–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.
Link: https://doi.org/10.1021/acsmaterialslett.4c01573
