Tuning Multi‐Active Sites in Ni(OH) ₂ Catalyst via V/Ru Doping for Ampere‐Level Upcycling of Polyethylene Terephthalate Plastic

ABSTRACT The electrochemical oxidation of ethylene glycol (EG), which is derived from polyethylene terephthalate (PET) plastic, into value‐added chemicals presents a promising strategy for mitigating plastic pollution. However, its industrial viability is significantly constrained by the low current density and the competing oxygen evolution reaction. Herein, we modify nickel layered double hydroxide (NiVRu‐LDH) through vanadium and ruthenium doping to enhance the current density while maintaining a high Faradaic efficiency (FE >90%) over a broad current density range (100–2000 mA/cm 2 ), surpassing those of pristine NiV‐LDH (100–1000 mA/cm 2 ) and Ni(OH) 2 (100–300 mA/cm 2 ). Experimental and theoretical investigations demonstrate that V modification serves two critical functions: accelerating catalyst reconstruction from Ni 2+ (OH) 2 to Ni 3+ OOH and enhancing EG adsorption. Furthermore, Ru atoms effectively promote *OH generation, thereby facilitating EG oxydehydrogenation to formic acid. The synergistic effect of multiple active sites can effectively promote the rapid oxidation and dehydrogenation reaction of EG, thereby significantly inhibiting the competing oxygen evolution side reaction, which is the key mechanism for achieving the generation of formic acid at ampere‐level current density.