Tailoring active sites of cerium and nitrogen Co-doped rhenium disulfide for enhanced hydrogen evolution reaction

Abstract

The construction of electrocatalysts with exceptional intrinsic activity and rich active sites has proven to be an effective strategy for remarkably enhancing the activity of the hydrogen evolution reaction (HER). Here, self-supporting cerium (Ce) and nitrogen (N)-doped rhenium disulfide nanosheets (denoted Ce,N-ReS₂) grown on carbon fiber paper have been successfully synthesized. Ce and N doping modulates the lattice irregularity and adjusts the electronic configuration of rhenium disulfide, resulting in reduced hydrogen adsorption/desorption energy and enhanced catalytic stability. The optimized Ce,N-ReS₂ electrocatalysts exhibit superior catalytic activities of 44/130 and 79/139 mV at 10/100 mA/cm² for HER in alkaline and acidic media, respectively, along with robust durability. Both experimental results and density functional theory calculations indicate that the electronic structure of ReS₂ can be significantly altered by strategically incorporating Ce and N into the lattice, which in turn optimizes the Gibbs free energy of HER intermediates and accelerates the electrochemical kinetics. This study provides a potentially effective approach for the design and optimization of innovative electrocatalysts involving the regulation of anion and cation dual-doping and architectural engineering.