1T-MoS(2)Nanosheets Coupled with CoS(2 )Nanoparticles: ElectronicModulation for Efficient Electrochemical Nitrogen Fixation

Electrocatalytic nitrogen reduction reaction (eNRR), a substitute process for theconventional Haber-Bosch for NH3production, has drawn tremendous attention due to its meritsin mild conditions, abundant reactant sources, low energy consumption, and environmentalprotection. However, electrocatalysts for eNRR are still subjected to low catalytic activity andselectivity. Herein, we constructed a CoS2/1T-MoS2heterostructure with CoS2nanoparticlesuniformly loaded on 1T-MoS2nanosheets and applied it as an eNRR electrocatalyst for thefirsttime. Theoretical calculation suggests that electron transfer from CoS2to 1T-MoS2across theircontact interface optimizes the local electronic structure of 1T-MoS2, where the electron-depletionregion near CoS2is in favor of accepting lone-pair electrons from N2to enable N2absorption, andthe electron-accumulation region near 1T-MoS2is conductive to break inert N???N triple bonds.Unlike pure 1T-MoS2, the potential-determining step (PDS) demonstrates a significantly lower energy barrier. In addition, the weakinteraction between CoS2/1T-MoS2and hydrogen discourages competitive hydrogen evolution reaction. As a result, CoS2/1T-MoS2exhibited noticeably improved eNRR activity and selectivity, with an NH3yield of 59.3 mu gh-1mg-1and a high Faradaic efficiency of26.6%