Electrocatalytic Upcycling of Plastic Waste to Organonitrogen Chemicals via Intercepting Carbon Intermediates

Transforming and repurposing plastic waste into valuable commodity chemical products is a sustainable strategy, which is beneficial for not only managing plastic waste but also fostering a circular plastic economy. Herein, we reported an electrocatalytic polyethylene terephthalate (PET) plastic waste upcycling to organonitrogen chemicals strategy over a MnO₂ (MnO₂/CFP) catalyst. The MnO₂/CFP catalyst is capable of mildly oxidizing PET plastic-waste-derived ethylene glycol (EG) to electrophilic carbon intermediates under near-neutral conditions, in which the in situ formed carbon intermediates were stabilized and further attacked by nitrogenous nucleophiles, leading to the successful formation of amides. As a result, formamide (FE and yield up to 10.86% and 0.030 mmol cm^-2 h^-1, respectively) was produced as the primary C-N coupling product with EG and ammonia (NH₃) as C and N sources, respectively. Furthermore, amides were synthesized with real-world PET plastic waste as the C source, indicating the potential practical application of this proof-of-concept work.