Abstract
The catalytic upcycling of plastic mixtures into H2 and carbon nanotubes (CNTs) represents a transformative strategy for advancing plastic management and the circular economy. Herein, an in-situ constructed high-performance FeNi/Ni/C catalyst combined with prompt microwave catalysis enables efficient conversion of LDPE-PVC, LDPE-HDPE-PP-PS-PVC-PTFE and landfilled waste mixture into valuable H2 and CNTs, resulting in near-quantitative atom economy (i.e., H2 and carbon efficiencies are nearly 100%) together with H2 and CNTs yields reaching >922 mmol g-1catalyst and >10600 mg g-1catalyst, respectively. Furthermore, this microwave catalysis strategy presents an excellent stability (>35 cycles) via Cl/F-based regeneration and energy efficiency (80% reduction vs. traditional thermal catalysis), alongside a high turnover number of 107.6 molcarbon mol-1NiFe. Fundamentally, the Ni species contribute to C-H breaking, and Fe is beneficial for CNT formation during plastic decomposition. Here, we show a cost-effective platform for upcycling of chlorinated/fluorinated plastic mixtures, aligning with resource circularity objectives.
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Acknowledgements
We thank Lei Kang for his help in theoretical calculations, and Tiancun Xiao provided the landfilled mixed plastics waste feedstock from the UK landfilled site. We thank the staff at SSRF BL17B of the National Facility for Protein Science in Shanghai (NFPS), Shanghai Advanced Research Institute, CAS, for providing technical support in X-ray absorption fine structure data collection and analysis. We appreciate eChemStore (www.echemstore.cn) for the techno-economic analysis. J. Z. and W. M. disclose support for the research of this work from the Funder of National Natural Science Foundation of China (52500198) and the National Key R&D Program of China (No. 2019YFA0708700). J. T. and J. Y. disclose support for the research of this work from the Funder of the Beijing Natural Science Foundation (F251045) and the National Natural Science Foundation of China (U23B20162).
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Zhao, J., Yang, J., Wang, D. et al. ~100% upcycling of chlorinated/fluorinated plastic mixtures to H2 and nanotubes over FeNi/Ni/C by microwave catalysis. Nat Commun (2026). https://doi.org/10.1038/s41467-026-73141-w
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DOI: https://doi.org/10.1038/s41467-026-73141-w
