<p>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 &gt;922 mmol g<sup>-1</sup><sub>catalyst</sub>&#xa0;and &gt;10600 mg g<sup>-1</sup><sub>catalyst</sub>, respectively. Furthermore, this microwave catalysis strategy presents an excellent stability (&gt;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.</p>

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~100% upcycling of chlorinated/fluorinated plastic mixtures to H2 and nanotubes over FeNi/Ni/C by microwave catalysis

  • Jun Zhao,
  • Jianlong Yang,
  • Duanda Wang,
  • Huanrong Zhang,
  • Qianqian Jia,
  • Lei Zhang,
  • Zhenguo An,
  • Mianqi Xue,
  • Haijiao Xie,
  • Wangjing Ma,
  • Lu Zhang,
  • Sui Zhao,
  • Junwang Tang

摘要

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.