Nearly 100% Valorization in Seconds: Transforming PET‐Metal Oxide Mixtures Into M ₁ O _x Clusters on rGO and Premium Syngas/Aromatics Products

ABSTRACT 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 (M 1 O 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 H 2 ), the aromatic fraction contains 22.84 mmol benzene, and the solid product is Zn 1 O 4 /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 Zn 1 O 4 /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 Zn 1 O 4 /rGO nanosheets exhibit excellent electrocatalytic performance for syngas production via CO 2 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.