关键词:
5-Hydroxymethylfurfural
Selective hydrogenation
Formic acid oxidation
Electrocatalyst
Bifunction
摘要:
The electrochemical hydrogenation(ECH)of 5-hydroxymethylfurfural(HMF)to 2,5-dihydroxymethylfuran(DHMF)represents a pivotal pathway for the electrocatalytic upgrading of biomass-based organic small molecules,offering significant reductions in energy consumption while producing value-added *** conversion of HMF to DHMF is challenging due to the high reduction potential and complex intermediates of HMF ECH under neutral ***,the total efficiency is hindered by sluggish anodic oxygen evolution reaction(OER)***,we report a synthesis of highly alloyed Pd-Pt bimetallene(Pd3Pt1 BML)for HMF ECH coupled with formic acid oxidation reaction(FAOR).Through a combination of in-situ Raman spectroscopy,electron paramagnetic resonance analysis,and theoretical calculations,we elucidate that the HMF adsorption on Pd atoms,strategically separated by Pt atoms,is weakened compared to pure Pd ***,Pt atoms serve as crucial providers of active hydrogen to neighboring Pd atoms,synergistically enhancing the reaction kinetics of HMF conversion with a Faradaic efficiency>93%.Meanwhile,the atomically dispersed Pt atoms endow Pd_(3)Pt_(1) BML with high electrochemical performance for the direct pathway of FAOR at the *** a result,a FAOR-assisted HMF ECH system equipped with bifunctional Pd3Pt1 BML achieves the energy-efficient conversion of HMF to DHMF at electrolysis voltage of 0.72 V at 10 mA cm^(–2).This work provides insights into the rational design of bifunctional catalysts featuring two distinct types of active sites for advanced energy electrocatalysis and ECH.