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<p>The valorization of plastic waste represents a major challenge of the 21st century due to its severe environmental impact. Here, we report a stepwise hydrogen spillover-constructed CuCo/CoO<sub>x</sub> catalyst that enables near-quantitative conversion of waste polyethylene terephthalate to <i>p</i>-xylene (&gt;99.9%), significantly outperforming the performance of various Cu- and Co-based catalysts as well as previously reported noble metal catalysts. The stepwise hydrogen spillover induces the formation of partially phase-transformed Co<sup>0</sup> species and abundant oxygen-vacancy-rich Co<sup>0</sup>/CoO<sub>x</sub> interfaces. The former enhances H<sub>2</sub> dissociation efficiency, while the latter facilitates C-O bond activation in polyethylene terephthalate and regulates substrate-product adsorption equilibria, synergistically contributing to the exceptional catalytic performance. The catalyst demonstrates broad applicability to more than 30 real-world polyester plastics. Furthermore, techno-economic analysis reveals significant reductions in CO<sub>2</sub> emissions and competitive processing costs. This breakthrough in near-quantitative polyethylene terephthalate conversion and stepwise hydrogen spillover-enabled active site construction offers valuable insights into plastic waste upcycling and the design of advanced heterogeneous catalysts.</p>

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Stepwise hydrogen spillover–engineered synergistic sites enable near-quantitative conversion of waste PET to p-xylene

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年1月28日

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  • Wenyi Ni,
  • Hongshun Ran,
  • Rui Wang,
  • Yifan Liu,
  • Pengfei Zhou,
  • Tao Guo,
  • Junjie Shan,
  • Zhuangzhuang Lai,
  • Beibei Liu,
  • Shi-Jun Liang,
  • Feng Miao,
  • Xinyi Cui,
  • Yaxuan Jing

摘要

The valorization of plastic waste represents a major challenge of the 21st century due to its severe environmental impact. Here, we report a stepwise hydrogen spillover-constructed CuCo/CoOx catalyst that enables near-quantitative conversion of waste polyethylene terephthalate to p-xylene (>99.9%), significantly outperforming the performance of various Cu- and Co-based catalysts as well as previously reported noble metal catalysts. The stepwise hydrogen spillover induces the formation of partially phase-transformed Co0 species and abundant oxygen-vacancy-rich Co0/CoOx interfaces. The former enhances H2 dissociation efficiency, while the latter facilitates C-O bond activation in polyethylene terephthalate and regulates substrate-product adsorption equilibria, synergistically contributing to the exceptional catalytic performance. The catalyst demonstrates broad applicability to more than 30 real-world polyester plastics. Furthermore, techno-economic analysis reveals significant reductions in CO2 emissions and competitive processing costs. This breakthrough in near-quantitative polyethylene terephthalate conversion and stepwise hydrogen spillover-enabled active site construction offers valuable insights into plastic waste upcycling and the design of advanced heterogeneous catalysts.