Lewis-Acid Engineering with Neodymium Promoters as Synergistic Nd-Ni Dual Sites for Enhanced Urea Oxidation

The sluggish kinetics of the urea oxidation reaction (UOR) are strongly associated with the high energy barriers required for the C-N cleavage and N-N coupling steps. While nickel-based catalysts are promising, their performance is limited by high operational potentials and structural instability. This work introduces neodymium (Nd) as a Lewis acid site promoter into a nickel-based framework to create Nd-Ni oxide catalysts. The strong Lewis acidity of Nd centers enhances urea adsorption and facilitates C-N cleavage and N-N coupling, while the significant electronegativity difference between Nd and Ni induces electronic redistribution for optimizing intermediate adsorption for UOR. As a result, the optimal catalyst demonstrates superior UOR performance, in which a low potential of 1.347 V is required to achieve 10 mA cm^-2 accompanied by excellent cycling stability. When integrated into a Zn-urea battery, it delivers a peak power density of 11.6 mW cm^-2. This study highlights the critical role of Lewis-acid engineering via rare-earth metal incorporation in restructuring reaction pathways, and offers a promising strategy for advancing renewable energy conversion.