电子结构不对称碳介导的Pd电荷重分布促进乙醇氧化反应OA

Pd-based materials as the promising catalysts for ethanol oxidation reaction(EOR)are still intrinsically limited by the surface electronic-structure trade-off between ethanol adsorption and CH3CO intermediate desorption.Herein,the Pd supported on N/S co-doped carbon(Pd@SNC)catalyst is synthesized,in which the doped S and N atoms could transfer moderate amounts electron to Pd,leading to opportune electron structure of Pd.Moreover,the moderate negative shift of d-band center demonstrate that the opportune Pd electron structure can strengthen adsorption of ethanol/OH-and promote the desorption of intermediate(CH3CO*),which may facilitate the kinetics.As a result,Pd@SNC exhibiting the highest catalytic activity for EOR(945.49 mA mgPd-1),surpassing to that of Pd@NC and Pd@C.Due to the fact that the electronic structure of Pd is properly regulated by co-doped N and S atoms,as shown by the theoretical calculation results,Pd@SNC exhibits the lowest reaction energy barrier of the dehydrogenation during the process of EOR.