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.
Li et al. (Sun,) studied this question.