In Situ Raman Study of Surface Reconstruction of FeOOH/Ni3S2 Oxygen Evolution Reaction Electrocatalysts.

Abstract

Construction of heterojunctions is an effective strategy to enhanced electrocatalytic oxygen evolution reaction (OER), but the structural evolution of the active phases and synergistic mechanism still lack in-depth understanding. Here, an FeOOH/Ni3S2 heterostructure supported on nickel foam (NF) through a two-step hydrothermal-chemical etching method is reported. In situ Raman spectroscopy study of the surface reconstruction behaviors of FeOOH/Ni3S2/NF indicates that Ni3S2 can be rapidly converted to NiOOH, accompanied by the phase transition from α-FeOOH to β-FeOOH during the OER process. Importantly, a deep analysis of Ni─O bond reveals that the phase transition of FeOOH can regulate the lattice disorder of NiOOH for improved catalytic activity. Density functional theory (DFT) calculations further confirm that NiOOH/FeOOH heterostructure possess strengthened adsorption for O-containing intermediates, as well as lower energy barrier toward the OER. As a result, FeOOH/Ni3S2/NF exhibits promising OER activity and stability in alkaline conditions, requiring an overpotential of 268mV @ 100mAcm-2 and long-term stability over 200h at a current density of 200mAcm-2. This work provides a new perspective for understanding the synergistic mechanism of heterogeneous electrocatalysts during the OER process.