Modulating electronic structure of Ni/carbon spherical nano-superstructures through transition metal-doping as highly efficient catalysts for hydrogen evolution reaction

The development of low-cost, high-performance electrocatalysts for hydrogen precipitation reactions is the key to solving the energy crisis. Metal organic framework (MOFs) with metal centers and organic ligands are one of the ideal materials for the preparation of non-precious metal carbon-based HER electrocatalysts. In this work, a series of transition metal-doped nano-superstructures carbon-based materials NiMC (M = Fe, Co, Cu) were designed and prepared by introducing different transition metal atoms using Ni-MOF as precursors. And the effect of transition metal doping on the electrocatalytic hydrogen precipitation performance of Ni-MOF has been systematically investigated. Nitrogen adsorption tests have shown that the NiFeC catalyst has the highest specific surface area. The overpotential was only 69 mV at a current density of 10 mA cm−2 in an alkaline electrolyte and exhibited excellent stability. Density functional theory (DFT) calculations show that the electronic interactions between Fe and Ni are tuned after Fe atom doping, which optimizes the hydrogen adsorption energy leading to the excellent HER catalytic performance of NiFeC.