Tandem methanolysis and catalytic transfer hydrogenolysis of polyethylene terephthalate to p-xylene over Cu/ZnZrOx catalysts DOI Creative Commons
Ryan Helmer, Siddhesh S. Borkar,

Aojie Li

et al.

Published: Aug. 28, 2024

We demonstrate a novel approach of utilizing methanol (CH3OH) for both the methanolysis polyethylene terephthalate (PET) to form dimethyl (DMT) at near-quantitative yields (~97%) and catalytic transfer hydrogenolysis (CTH) DMT p-xylene (PX, ~63% 240 °C 16 h) on reducible ZnZrOx supported Cu catalyst (i.e., Cu/ZnZrOx). Pre- post-reaction surface bulk characterization, along with density functional theory (DFT) computations, explicate role metal-support interface Cu/ZnZrOx in providing active sites activation CH3OH facilitating lower free-energy pathway dehydrogenation hydrogenolysis, compared redox-neutral SiO2 support. DFT calculations further reveal that rate-determining step CTH is cleavage C-O linkages –(C=O)-OR) DMT. Loading studies thermodynamic showed that, under reaction conditions, gas phase, rather than liquid critical Interestingly, was also effective C-C bonds (compared PET) waste polycarbonate (PC), largely forming xylenol (~38%) methyl isopropyl anisole (~42%) demonstrating versatility this toward valorizing wide range condensation polymers.

Language: Английский

Tandem methanolysis and catalytic transfer hydrogenolysis of polyethylene terephthalate to p-xylene over Cu/ZnZrOx catalysts DOI Creative Commons
Ryan Helmer, Siddhesh S. Borkar,

Aojie Li

et al.

Published: Aug. 28, 2024

We demonstrate a novel approach of utilizing methanol (CH3OH) for both the methanolysis polyethylene terephthalate (PET) to form dimethyl (DMT) at near-quantitative yields (~97%) and catalytic transfer hydrogenolysis (CTH) DMT p-xylene (PX, ~63% 240 °C 16 h) on reducible ZnZrOx supported Cu catalyst (i.e., Cu/ZnZrOx). Pre- post-reaction surface bulk characterization, along with density functional theory (DFT) computations, explicate role metal-support interface Cu/ZnZrOx in providing active sites activation CH3OH facilitating lower free-energy pathway dehydrogenation hydrogenolysis, compared redox-neutral SiO2 support. DFT calculations further reveal that rate-determining step CTH is cleavage C-O linkages –(C=O)-OR) DMT. Loading studies thermodynamic showed that, under reaction conditions, gas phase, rather than liquid critical Interestingly, was also effective C-C bonds (compared PET) waste polycarbonate (PC), largely forming xylenol (~38%) methyl isopropyl anisole (~42%) demonstrating versatility this toward valorizing wide range condensation polymers.

Language: Английский

Citations

1