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Electrocatalytic upcycling of polyethylene terephthalate (PET) waste plastics into value-added chemicals offers a promising strategy to address environmental pollution. However, the development of efficient electrocatalysts capable of operating under industrial-level current densities remains a significant challenge. In this study, we report an electrochemical reconstruction strategy to fabricate Ni2+-doped CoOOH nanosheet arrays directly on nickel foam (NF), enabling highly efficient conversion of PET-derived ethylene glycol (EG) into formate at high current densities. Systematic investigations, including in situ spectroscopic analysis, reveal that Ni2+ doping not only enhances the adsorption of EG molecules on the catalyst surface but also accelerates the formation of reactive *OH intermediates, thereby improving the reaction kinetics of C–C bond cleavage, ultimately promoting efficient formate production. Specifically, the optimized Ni2+-CoOOH3/NF catalyst achieves an industrial-level current density of 500 mA·cm-2 at an ultralow potential of 1.38 V vs. RHE, with a Faradaic efficiency exceeding 90% across a broad current density range of 100–500 mA·cm−2. Furthermore, in a practical two-electrode electrolyzer, the Ni2+-CoOOH3/NF delivers a high formate yield of 7.10 mmol·h−1·cm−2 at 900 mA·cm−2, along with excellent long-term operational stability.

This is an open access article under the terms of the Creative Commons Attribution 4.0 International License (CC BY 4.0, https://creativecommons.org/licenses/by/4.0/).
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