2D FeS_x Nanosheets by Atomic Layer Deposition: Electrocatalytic Properties for the Hydrogen Evolution Reaction

Abstract 2‐dimensional FeS x nanosheets of different sizes are synthesized by applying different numbers of atomic layer deposition (ALD) cycles on TiO 2 nanotube layers and graphite sheets as supporting materials and used as an electrocatalyst for the hydrogen evolution reaction (HER). The electrochemical results confirm electrocatalytic activity in alkaline media with outstanding long‐term stability (>65 h) and enhanced catalytic activity, reflected by a notable drop in the initial HER overpotential value (up to 26 %). By using a range of characterization techniques, the origin of the enhanced catalytic activity was found to be caused by the synergistic interplay between in situ morphological and compositional changes in the 2D FeS x nanosheets during HER. Under the application of a cathodic potential in alkaline media, the as‐synthesized 2D FeS x nanosheets transformed into iron oxyhydroxide‐iron oxysulfide core‐shell nanoparticles, which exhibited a higher active catalytic surface and newly created Fe‐based HER catalytic sites.