Interface Charge Distribution Engineering of Pd-CeO₂ /C for Efficient Carbohydrazide Oxidation Reaction

Carbohydrazide electrooxidation reaction (COR) is a potential alternative to oxygen evolution reaction in water splitting process. However, the sluggish kinetics process impels to develop efficient catalysts with the aim of the widespread use of such catalytic system. Since COR concerns the adsorption/desorption of reactive species on catalysts, the electronic structure of electrocatalyst can affect the catalytic activity. Interface charge distribution engineering can be considered to be an efficient strategy for improving catalytic performance, which facilitates the cleavage of chemical bond. Herein, highly dispersed Pd nanoparticles on CeO₂ /C catalyst are prepared and the COR catalytic performance is investigated. The self-driven charge transfer between Pd and CeO₂ can form the local nucleophilic and electrophilic region, promoting to the adsorption of electron-withdrawing and electron-donating group in carbohydrazide molecule, which facilitates the cleavage of C-N bond and the carbohydrazide oxidation. Due to the local charge distribution, the Pd-CeO₂ /C exhibits superior COR catalytic activity with a potential of 0.27 V to attain 10 mA cm^-2 . When this catalyst is used for energy-efficient electrolytic hydrogen production, the carbohydrazide electrolysis configuration exhibits a low cell voltage (0.6 V at 10 mA cm^-2 ). This interface charge distribution engineering can provide a novel strategy for improving COR catalytic activity.