Our
civilization relies on synthetic polymers for all aspects of
modern life; yet, inefficient recycling and extremely slow environmental
degradation of plastics are causing increasing concern about their
widespread use. After a single use, many of these materials are currently
treated as waste, underutilizing their inherent chemical and energy
value. In this study, energy-rich polyethylene (PE) macromolecules
are catalytically transformed into value-added products by hydrogenolysis
using well-dispersed Pt nanoparticles (NPs) supported on SrTiO3 perovskite nanocuboids by atomic layer deposition. Pt/SrTiO3 completely converts PE (Mn =
8000–158,000 Da) or a single-use plastic bag (Mn = 31,000 Da) into high-quality liquid products, such
as lubricants and waxes, characterized by a narrow distribution of
oligomeric chains, at 170 psi H2 and 300 °C under
solvent-free conditions for reaction durations up to 96 h. The binding
of PE onto the catalyst surface contributes to the number averaged
molecular weight (Mn) and the narrow polydispersity
(Đ) of the final liquid product. Solid-state
nuclear magnetic resonance of 13C-enriched PE adsorption
studies and density functional theory computations suggest that PE
adsorption is more favorable on Pt sites than that on the SrTiO3 support. Smaller Pt NPs with higher concentrations of undercoordinated
Pt sites over-hydrogenolyzed PE to undesired light hydrocarbons.