Influence of Pt/Ru anodic ratio on the valorization of ethanol by PEM electrocatalytic reforming towards value-added products

摘要

The ethanol electro-reforming process was studied over PtRu/C catalysts synthesized by the modified polyol method with different compositions.In particular,this work reports the influence of anodic Pt:Ru ratio(5:1,2:1 and 1:2)on the organic product distribution(acetaldehyde,acetic acid and ethyl acetate)and pure hydrogen generation at different current densities operation levels.Physicochemical characterization of the catalysts was made by X-ray diffraction(XRD),temperature-programmed reduction(TPR)and N_(2) adsorption-desorption measurements.XRD patterns showed that Ru is introduced into the Pt structure,forming an alloy between both metals.Also,the degree of alloy was higher by increasing the Ru amounts.From TPR profiles Pt was found to be properly reduced while Ru was both in metallic state and forming RuO2.The electrochemical behaviour of each catalyst towards ethanol electroreforming process was investigated through electrochemical techniques in a half cell and a single proton exchange membrane(PEM)cell systems.An intermediate Pt:Ru ratio was found to result in high current density and electrochemical surface area(ECSA)values along with lower amounts of adsorbed species.Also,Ru addition seems to diminish the degree of degradation of the catalyst.Based on characterization and in agreement with essays carried out in a PEM cell at mild conditions(80℃ and 1 atm),PtRu/C 2:1 anode provided the best electrocatalytic results in terms of current density(740 mA cm^(-2)),hydrogen production and selectivity toward acetic acid(up to 15%apart from acetaldehyde and ethyl acetate)while requiring the lowest energy consumption.