Ag engineered NiFe-LDH/NiFe2O4 Mott-Schottky heterojunction electrocatalyst for highly efficient oxygen evolution and urea oxidation reactions

Efficient and durable electrocatalysts with sufficient active sites and high intrinsic activity are essential for advancing energy-saving hydrogen production technology. In this study, a Mott-Schottky heterojunction electrocatalyst with Ag nanoparticles in-situ grown on NiFe layered double hydroxides (NiFe-LDH)/NiFe2O4 nanosheets (Ag@NiFe-LDH/NiFe2O4) were designed and successfully synthesized through a hydrothermal process and subsequent spontaneous redox reaction. The in-situ growth of metallic Ag on semiconducting NiFe-LDH/NiFe2O4 triggers a strong electron interaction across the Mott-Schottky interface, leading to a significant increase in both the intrinsic catalytic activity and the electrochemical active surface area of the heterojunction electrocatalyst. As a result, the Ag@NiFe-LDH/NiFe2O4 demonstrates impressive oxygen evolution reaction (OER) performance in alkaline KOH solution, achieving a low overpotential of 249 mV at 100 mA cm-2 and a Tafel slope of 42.79 mV dec-1. When the self-supported Ag@NiFe-LDH/NiFe2O4 is coupled with the Pt/C electrocatalyst, the alkaline electrolyzer reaches a current density of 10 mA cm-2 at a cell voltage of only 1.460 V. Furthermore, X-ray photoelectron spectroscopy and in-situ Raman analysis reveal that the Ni(Fe)OOH is the possible active phase for OER in the catalyst. In addition, when employed for UOR catalysis, the Ag@NiFe-LDH/NiFe2O4 also displays intriguing activity with an ultralow potential of 1.389 V at 50 mA cm-2. This work may shed light on the rational design of multiple-phase heterogeneous electrocatalysts and demonstrate the significance of interface engineering in enhancing catalytic performance.