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

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