摘要
Currently,the most efficient electrocatalyst for the hydrogen evolution reaction(HER)in water dissociation is Pt-based catalyst.Unfortunately,the high cost and less than perfect efficiency hinder wide-range industrial/technological applications.Here,by controlling the treatment temperature of tris(2,2-bipyridine)ruthenium dichloride hexahydrate,synthesis of compounds with novel ruthenium single/dual atoms(Ru S/DAs)mixed with Ru nanoclusters(Ru S/DAs+Ru NCs)and supported by carbon dots is demonstrated.These compounds are shown to be highly efficient and competitive catalysts for hydrogen evolution.Ru S/DAs+Ru NCs exhibit very high activity,with overpotentials of 15 and 40mV at a current density of 10mA/cm2 in 1.0mol/L KOH and 0.5mol/L H2SO4,respectively.Furthermore,the composites are found to possess outstanding stability and rapid HER kinetics.X ray absorption fine structure analysis,supported by density functional theory calculations,shows charge rearrangement in single-atomic Ru,and the Ru dual sites promote active hydrogen adsorption and recombination.Ru S/DAs and Ru NCs demonstrate high electroactivity due to the electroactive Ru 4d orbitals.The introduction of Ru NCs activates the carbon support,providing a high electronic conductivity to transfer electrons from Ru NCs to Ru S/DAs,and facilitates water dissociation for the HER process.
基金
supported by the National Natural Science Foundation of China(21905253,51973200,92061201)
the China Postdoctoral Science Foundation(2018M640681,2019T120632)
Natural Science Foundation of Henan(202300410372).
