Surface Ligand Modification on Ultrathin Ni(OH)₂ Nanosheets Enabling Enhanced Alkaline Ethanol Oxidation Kinetics

The ethanol oxidation reaction (EOR) is an economical pathway in many electrochemical systems for clean energy, such as ethanol fuel cells and the anodic reaction in hydrogen generation. Noble metals, such as platinum, are benchmark catalysts for EOR owing to their superb electrochemical capability. To improve sustainability and product selectivity, nickel (Ni)-based electrocatalysts are considered promising alternatives to noble-metal EOR. Although Ni-based electrocatalysts are relieved from intermediate poisoning, their performances are largely limited by their relatively high onset potential. Therefore, the EOR usually competes with the oxygen evolution reaction (OER) at working potentials, resulting in a low EOR efficiency. Here, we demonstrate a strategy to modify the surface ligands on ultrathin Ni(OH)₂ nanosheets, which substantially improved their catalytic properties for the alkaline EOR. Chemisorbed octadecylamine ligands could create an alcoholophilic layer at the nanosheet surface to promote alcohol diffusion and adsorption, resulting in outstanding EOR activity and selectivity over the OER at higher potential. These non-noble-metal-based 2D electrocatalysts and surface ligand engineering showcase a promising strategy for achieving high-efficiency electrocatalysis of EOR in many practical electrochemical processes.