Boosted Photoreforming of Plastic Waste viaDefect-Rich NiPS3Nanosheets

Sustainable conversion of plastic waste to mitigate environmental threats and reclaim waste value is important. Ambient-condition photoreforming is practically attractive to convert waste to hydrogen (H2); however, it has poor performance because of mutual constraint between proton reduction and substrate oxidation. Here, we realize a cooperative photoredox using defect-rich chalcogenide nanosheet-coupled photocatalysts, e.g., d-NiPS3/CdS, to give an ultrahigh H2evolution of ∼40 mmol gcat–1h–1and organic acid yield up to 78 μmol within 9 h, together with excellent stability beyond 100 h in photoreforming of commercial waste plastic poly(lactic acid) and poly(ethylene terephthalate). Significantly, these metrics represent one of the most efficient plastic photoreforming reported. In situultrafast spectroscopic studies confirm a charge transfer-mediated reaction mechanism in which d-NiPS3rapidly extracts electrons from CdS to boost H2evolution, favoring hole-dominated substrate oxidation to improve overall efficiency. This work opens practical avenues for converting plastic waste into fuels and chemicals.