Enhancing plastic photoreforming by modulating active radicals via lattice-matched heterointerfaces for frustrated Lewis pair formation

The sustained oxidation of ethylene glycol (EG) is essential for polyethylene terephthalate (PET) decomposition, necessitating effective photocatalyst heterojunctions to generate specific free radicals for EG deoxidation. Herein, we fabricate a lattice-matched SiC/LaOCl heterojunction via molten-salt electrochemical biorefining for PET upcycling to value-added acetate and glycolate with H 2 . SiC/LaOCl not only improves photogenerated charge carrier separation via a low energy barrier for PET decomposition but also features frustrated Lewis pairs (FLPs) that form undercoordinated La atoms and adjacent oxygen vacancies to steer oxidation mechanisms from •OH-mediated cleavage to a C α -centered radical pathway, achieving 64.71% acetate selectivity. Life-cycle assessment confirms that photoreforming PET reduces CO 2 emissions by 45% compared to thermal catalysis systems, and techno-economic analysis indicates that the SiC/LaOCl photocatalyst requires only 33 hours of operation to recoup its production cost. This study advances photoreforming for carbon-neutral plastic upcycling by integrating PET depolymerization with selective C–O/C–C activation.