Dynamic reconstruction Engineering of Nickel(II) carbonate hydroxide for enhanced electrocatalytic alcohol oxidation

The selective electrocatalytic oxidation of alcohols (EOA) to aldehydes under weak alkaline conditions offers sustainable synthetic routes. However, a deficiency in basicity inevitably leads to diminished electrocatalytic efficiency, and the dynamic reconstruction mechanism of the electrocatalyst remains insufficiently researched. Herein, the NiMoO x -COOH electrocatalyst/4-acetamido-TEMPO (ACT) synergistic system was employed for the efficient EOA under weak alkaline. In situ studies reveal electric double layer-driven metal/ligand co-leaching induces in situ dissolution-redeposition of metal, forming active Ni 2 (CO 3 )(OH) 2 . Experimental and Density functional theory (DFT) studies confirm a synergistic electrocatalytic mechanism between NiMoO x -COOH and ACT. The reconstructed Ni 2 (CO 3 )(OH) 2 promotes ACTH surface adsorption, thereby facilitating the turnover cycle of ACT. Therefore, outstanding EOA electrocatalytic performance has been achieved (500 mA/cm 2 , 96 % high yield, maintaining 30 cycles for benzyl alcohol oxidation, 15 substrate examples and 100 g scales synthesis). This work offers a promising approach to achieving high-performance EOA under weak alkaline.