~100% upcycling of chlorinated/fluorinated plastic mixtures to H<sub>2</sub> and nanotubes over FeNi/Ni/C by microwave catalysis.

Zhao, Jun; Yang, Jianlong; Wang, Duanda; Zhang, Huanrong; Jia, Qianqian; Zhang, Lei; An, Zhenguo; Xue, Mianqi et al. · Nat Commun · 2026

basic_science · Level V

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Abstract

The catalytic upcycling of plastic mixtures into H<sub>2</sub> 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 H<sub>2</sub> and CNTs, resulting in near-quantitative atom economy (i.e., H<sub>2</sub> and carbon efficiencies are nearly 100%) together with H<sub>2</sub> and CNTs yields reaching >922 mmol g<sup>-1</sup><sub>catalyst</sub> and >10600 mg g<sup>-1</sup><sub>catalyst</sub>, 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 mol<sub>carbon</sub> mol<sup>-1</sup><sub>NiFe</sub>. 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.