Deep Reconstruction of the NiFeSP Nanosheet Catalyst for Large Current-Density Water Oxidation

Evidence shows that the crucial factor in achieving efficient water electrolysis for hydrogen production is the design and synthesis of electrocatalysts that exhibit both high performance and cost-effectiveness for the oxygen evolution reaction (OER). Herein, the NiFeSP nanosheets were facilely prepared on a Ni foam (NF) substrate through a cost-effective electrodeposition method. The electrode structure composed of nanosheets offers a high density of active sites and superior electrical conductivity, thereby enhancing the efficiency of the OER. In addition, the NiFeSP/NF-600 nanosheets exhibit superhydrophilic and superaerophobic characteristics, which effectively enhance the mass-transfer process by facilitating the penetration of electrolytes and enabling rapid release of gas bubbles. Consequently, NiFeSP/NF-600 demonstrates superior electrocatalytic efficacy for OER, exhibiting an overpotential of 292 mV at a high current density of 500 mA cm^-2 as well as an exceptional long-term durability of 100 h. More importantly, the rapid reconstruction of FeOOH and NiOOH species from NiFeSP/NF-600 may be the true active species for OER, which is revealed utilizing in situ Raman spectroscopy in conjunction with ex situ characterization. This study not only offers an ideal "pre-catalyst" for an extremely effective OER but also offers a thorough understanding of the mechanism underlying the structural evolution of electrocatalysts and the identification of their actual active sites.