Zhu Yue, Mao Zhouying, Wu Weixiang, Han Buxing, Mei Qingqing
Institute of Environment Science and Technology, College of Environmental and Resource Sciences, Zhejiang University, Hangzhou 310058, China.
Innovation Center of Yangtze River Delta, Zhejiang University, Jiaxing, Zhejiang 311400, China.
J Am Chem Soc. 2025 Mar 26;147(12):10662-10677. doi: 10.1021/jacs.5c01209. Epub 2025 Mar 13.
The partial hydrogenation of waste polyethylene terephthalate (PET) offers a great opportunity to produce valuable chemicals, yet achieving precise catalytic control remains challenging. Herein, for the first time, we realized one-pot selective hydrogenation of waste PET to -toluic acid (-TA) with a record-high yield of 53.4%, alongside a 36.4% yield of -xylene (PX), using a specially designed PtW/MCM-48 catalyst. Mechanistic investigations revealed that the exceptional catalytic performance arises from synergistic interaction between Pt nanoparticles and WO species. Low-valent WO enhances Pt dispersion, while Pt stabilizes WO as low-polymerized polytungstates. The moderate acidity of PtW/MCM-48 ensures controlled desorption of -TA, preventing overhydrogenation to PX. The catalyst demonstrated robust performance with real-world PET waste. Life cycle assessment and technical and economic evaluation further highlight its practical feasibility. This study establishes a sustainable pathway for PET chemical upcycling and provides a framework for designing advanced catalysts for selective hydrogenation reactions, addressing critical challenges in circular chemistry and plastic waste management.
废弃聚对苯二甲酸乙二酯（PET）的部分氢化反应为生产有价值的化学品提供了巨大机遇，但实现精确的催化控制仍然具有挑战性。在此，我们首次使用特别设计的PtW/MCM-48催化剂，实现了废弃PET一锅法选择性氢化为对苯二甲酸（TA），产率高达53.4%，创历史新高，同时对二甲苯（PX）的产率为36.4%。机理研究表明，优异的催化性能源于Pt纳米颗粒与WO物种之间的协同相互作用。低价态的WO增强了Pt的分散性，而Pt将WO稳定为低聚多钨酸盐。PtW/MCM-48适度的酸度确保了TA的可控脱附，防止过度氢化为PX。该催化剂对实际的PET废料表现出稳健的性能。生命周期评估以及技术和经济评估进一步凸显了其实际可行性。本研究为PET化学升级循环建立了一条可持续途径，并为设计用于选择性氢化反应的先进催化剂提供了框架，解决了循环化学和塑料废料管理中的关键挑战。
