The work links plastic waste remediation with high‑value chemical production, offering a scalable, low‑energy pathway for renewable formic acid synthesis. It demonstrates that 2D MOF architecture can dramatically improve electrocatalytic performance, influencing future catalyst design across the green chemistry sector.
The surge in single‑use PET packaging has created a pressing need for circular solutions that go beyond mechanical recycling. Converting PET into two‑dimensional metal‑organic frameworks leverages the polymer’s aromatic backbone as a ligand source, producing ultrathin sheets with abundant active edges. These 2D MOFs inherit the high surface‑area benefits of nanomaterials while retaining the tunable electronic environments characteristic of coordination chemistry, positioning them as attractive platforms for electrocatalytic applications that demand both activity and durability.
In the reported 2D‑CoNi‑PET catalyst, nickel atoms act as electronic promoters, oxidizing adjacent cobalt centers to higher valence states. This electronic modulation reduces the deprotonation barrier for ethylene glycol, shifting the EGOR onset to just 1.41 V versus RHE. Moreover, the diminished electron density on cobalt strengthens adsorption of oxygen‑containing intermediates, accelerating the reaction cascade that converts ethylene glycol to formic acid. Comparative experiments reveal that the planar geometry of the nanosheets facilitates a more efficient adsorption‑reaction chain than bulkier 3D MOFs, translating into a 91 % formic‑acid selectivity at industrially relevant current densities.
The implications extend beyond a single reaction. Achieving high Faradaic efficiency and selectivity at low overpotential demonstrates that plastic‑derived electrocatalysts can rival, or even surpass, conventional precious‑metal systems. This opens avenues for decentralized, renewable production of platform chemicals such as formic acid, reducing dependence on fossil‑based feedstocks. Future research may explore other waste polymers as MOF precursors, expand the metal palette, and integrate these catalysts into flow‑cell architectures, accelerating the transition toward a circular, electrochemical economy.
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