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Revealing Electronic Effect in Mesoporous Medium-Entropy Alloy for Promoting Electrocatalytic Upcycling of
Ziqiang Wang1, Jiale Song1, Jiabing Geng1
1State Key Laboratory of Green Chemical Synthesis and Conversion, Zhejiang Key Laboratory of Surface and Interface Science and Engineering for Catalysts, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, P. R. China.
Abstract:
The electrochemical valorization of polyethylene terephthalate (PET) plastic waste into high-value C2 products represents an attractive route for waste resource reutilization, and it is critical to identify advanced catalysts for PET-derived ethylene glycol oxidation reaction (EGOR) with high activity and selectivity. Herein, a mesoporous PtPdRuOs medium-entropy alloy (MEA) film on Ni foam (MEA-mPtPdRuOs/NF) is reported for electrosynthesis of glycolic acid (GA) from PET-derived ethylene glycol (EG), accompanying with cogeneration of hydrogen. MEA-mPtPdRuOs/NF demonstrates optimized Faradaic efficiency (95.2%) for GA production in PET hydrolysate. Experimental and theoretical analyses reveal a synergistic catalytic effect of the MEA in highly efficient EG-to-GA conversion, in which the Pt/Pd sites are responsible for the activation of EGOR intermediates and Os/Ru sites are contributed to water dissociation and *OH adsorption. Furthermore, the optimized electronic effect can reduce the EGOR energy barrier and enhance the C-C bond energy in key *OC-CH2OH intermediates, resulting in a higher performance for EG-to-GA conversion. In addition, the easy removal of poisonous CO species and high corrosion resistance make MEA-mPtPdRuOs/NF more stable for EGOR. This study proposes the rational design of a mesoporous MEA for the coproduction of valuable GA and H2 via waste PET electroupcycling.
