Defective Fe3GeTe2 monolayer as a promising electrocatalyst for spontaneous nitrogen reduction reaction

Abstract

The vital role of the spin polarization in the electrocatalytic N₂ reduction reaction (eNRR) stimulates us to explore the potential of the newly discovered two-dimensional (2D) vdW ferromagnetic materials as NRR electrocatalysts. Here, using density functional theory (DFT) computations, we report the first theoretical prediction that the single-layer defective Fe₃GeTe₂ acts as a 2D ferromagnetic material toward the NRR with outstanding electrocatalytic activity and high selectivity. Notably, all six hydrogenation steps are exothermic and spontaneous. The highly centralized spin-polarization on the exposed Fe₄ center in defective Fe₃GeTe₂ leads to strong backdonation and substantial activation of the NN triple bond. Moreover, the metallic character of the defective Fe₃GeTe₂ ensures high-speed transport of carriers. This work not only provides a quite promising electrocatalyst for the NRR but also promotes the application of emerging 2D ferromagnets in the field of energy conversion.