Nearly 100% Valorization in Seconds: Transforming PET-Metal Oxide Mixtures Into M₁O_x Clusters on rGO and Premium...

The efficient recycling of polyethylene terephthalate (PET) is often hindered by challenges such as low-value products, limited processing capacity, prolonged reaction times, and incomplete carbon conversion. Here, we develop a large-scale, ultrafast Joule-assisted reformation strategy that achieves nearly 100% valorization of physical mixtures containing 10 g of PET waste and metal oxides within seconds. This process converts more than 30% of the carbon into single-metal-atom oxide clusters supported on reduced graphene oxide (M₁O_x/rGO) nanosheets, while transforming the remaining carbon into high-value syngas and aromatic compounds. When applied to a physical mixture of PET waste and commercial ZnO, the gaseous products consist mainly of syngas (88.91 mmol CO and 41.85 mmol H₂), the aromatic fraction contains 22.84 mmol benzene, and the solid product is Zn₁O₄/rGO nanosheets. Synchrotron-radiation X-ray absorption fine structure and X-ray emission spectroscopy analyses confirm a four-coordinate oxygen environment around the Zn center in the as-synthesized Zn₁O₄/rGO nanosheets. The PET reformation pathway was monitored using quasi-in situ Fourier transform infrared spectroscopy and quasi-in situ gas chromatography/mass spectrometry, and ab initio molecular dynamics simulations revealed a fragmentation-annulation mechanism. The resulting Zn₁O₄/rGO nanosheets exhibit excellent electrocatalytic performance for syngas production via CO₂ reduction at an industrial-level current density of 400 mA cm^-2. This work establishes a new paradigm for the near-complete valorization of PET waste into high-value products.