Self-Evolving PET-Induced Carbon Nanotube Modulated Ni Nanocomposites for Efficient PET-to-H2 Production

Abstract Upcycling polyethylene terephthalate (PET) into H2-rich syngas offers a route for plastic pollution mitigation and green energy production yet remains constrained by low efficiency and catalyst deactivation. Here we report a carbon nanotube (CNT)-modulated catalytic strategy integrating PET decomposition with steam reforming. PET was first upcycled into CNT-modulated Ni nanocomposites, where PET-derived CNTs acted as structural and electronic bridges linking Ni nanoparticles (NPs) with the oxide support. Among catalysts evaluated in decomposition-catalytic steam reforming (DCSR), CNT-modulated Ni NPs anchored on γ-Al2O3 nanosheets (Ni NPs@PET-CNTs/γ-Al2O3) achieved a H2-rich syngas yield of 141.74 mmol/gPET (3175 mL/gPET), with excellent stability and self-regeneration under continuous operation. Mechanistic analysis revealed that the synergy of Ni0, PET-derived CNTs, and γ-Al2O3 underpinned enhanced activity and durability. This work establishes a paradigm where plastic waste acts as a carbon feedstock and catalyst modulator, enabling scalable PET upcycling toward sustainable H2-rich syngas production and circular carbon utilization.