An Electron Transfer Mediated Mechanism for Efficient Photoreforming of Waste Plastics Using a Ni<sub>3</sub>S<sub>4</sub>/ZnCdS Heterojunction
Zehao Ma, Shaoqi Zhan, Yule Zhang, Yule Zhang, Artem V. Kuklin, Yinxiang Chen, Ying‐Wu Lin, Han Zhang, Xiaohui Ren, Hans Ågren, Zhang Ye, Zhang Ye
Abstract
Abstract The oxidative degradation of plastics in conjunction with the production of clean hydrogen (H 2 ) represents a significant challenge. Herein, a Ni 3 S 4 /ZnCdS heterojunction is rationally synthesized and employed for the efficient production of H 2 and high‐selectivity value‐added chemicals from waste plastic. By integrating spectroscopic analysis techniques with density functional theory (DFT) calculations, a solely electron transfer‐mediated reaction mechanism is confirmed, wherein Ni 3 S 4 extracts electrons from ZnCdS (ZCS) to promote the spatial segregation of photogenerated electrons and holes, which not only facilitates H 2 production but also maintains the high oxidation potential of holes on the ZCS surface, favoring hole‐dominated plastic oxidation. Notably, the catalyst exhibited efficient H 2 production rates as high as 27.9 and 17.4 mmol g −1 h −1 , along with a selectivity of 94.2% and 78.3% in the liquid product toward pyruvate and acetate production from polylactic acid (PLA) and polyethylene terephthalate (PET), respectively. Additionally, carbon yields of 26.5% for pyruvate and 2.2% for acetate are measured after 9 h of photoreforming, representing the highest values reported to date. Overall, this research presents a promising approach for converting plastic waste into H 2 fuel and high‐selectivity valuable chemical products, offering a potential solution to the growing issue of “ White Pollution ”.