Interlayer ligand engineering of β-Ni(OH) 2 for oxygen evolution reaction

Oxygen evolution reaction (OER) is a bottleneck process for many electrochemical devices due to the sluggish kinetics, for which advanced electrocatalysts should be carefully designed. Nickle-based materials have been extensively studied to catalyze OER. However, their performances are still below the expectation and the active sites are often controversial. Herein, we have successfully modulated the electronic and surface properties of layered •-Ni(OH)2 by the interlayer ligand engineering, aiming to design novel efficient electrocatalysts and unveil the catalysis mechanism. By one-step solvothermal reaction, alkoxyl substituted •-Ni(OH)2 with variable interlayer distances is obtained, and the ethoxyl substituted one (NiEt) shows great potential for efficient OER. With the assistance of powder X-ray diffraction and crystalline structure computational simulation, the formula of alkoxyl substituted •-Ni(OH)2 are determined. Operando X-ray absorption spectroscopy studies combined with ex-situ analyses revealed that the critical active species of NiEt is formed via hydroxylation and subsequent de-protonation, with high valent Niδ+ (3<δ≤3.66). The corresponding catalytic reaction pathway and mechanism are proposed.