Abstract
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.
Data availability
Relevant data supporting the key findings of this study are available within the article and the Supplementary Information file. All raw data generated during the current study are available from the corresponding authors upon request. Source data are provided with this paper.
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Acknowledgments
This work was supported financially by the National Natural Science Foundation of China (22572083) (Y. J.), the Fundamental Research Funds for the Central Universities (491914380001 (Y. J., J. S., X. C.), 491914380008 (Y. J., X. C.)), Nanjing University International Collaboration Initiative (X. C.), Independent research project of State Key Laboratory of Water Pollution Control and Green Resource Recycling (Y. J.), and start-up funding for high-level talent at Nanjing University (491916002207) (Y. J.). We thank the BL11U beamlines (https://cstr.cn/31131.02.HLS.CSS) of the Catalysis and Surface Science Endstation in the National Synchrotron Radiation Laboratory (NSRL) in Hefei (https://cstr.cn/31131.02.HLS) for providing beam time, technical support and assistance in data collection and analysis to support this work.
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Y.J., X.C., F.M., and S.L. conceived and supervised the project. Y.J., W.N., and H.R. designed the experiments. W.N., H.R., Y.L., P.Z., T.G., and J.S. conducted the experiments and analyzed the data. Z.L. performed the DTF calculations. W.N., H.R., and R.W. performed the LCA and TEA. W.N. wrote the paper. Y.J., X.C., B.L., W.N., and H.R. revised the manuscript. All authors participated in discussions.
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Ni, W., Ran, H., Wang, R. et al. Stepwise hydrogen spillover–engineered synergistic sites enable near-quantitative conversion of waste PET to p-xylene. Nat Commun (2026). https://doi.org/10.1038/s41467-026-68990-4
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DOI: https://doi.org/10.1038/s41467-026-68990-4
