Boosted Photoreforming of Plastic Waste via Defect-Rich NiPS3 Nanosheets

• Published in: Journal of the American Chemical Society 2023-03, Vol.145 (11), p.6410-6419
• Main Authors: Zhang, Shuai, Li, Haobo, Wang, Lei, Liu, Jiandang, Liang, Guijie, Davey, Kenneth, Ran, Jingrun, Qiao, Shi-Zhang
• Format: Article
• Language: English
• ISSN: 0002-7863; 1520-5126
• DOI: 10.1021/jacs.2c13590

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 H2 evolution of ∼40 mmol gcat –1 h–1 and 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 situ ultrafast spectroscopic studies confirm a charge transfer-mediated reaction mechanism in which d-NiPS3 rapidly extracts electrons from CdS to boost H2 evolution, favoring hole-dominated substrate oxidation to improve overall efficiency. This work opens practical avenues for converting plastic waste into fuels and chemicals.