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