Polyethylene Terephthalate Deconstruction Catalyzed by a Carbon-Supported Single-Site Molybdenum-Dioxo Complex

Angew Chem Int Ed Engl. 2020 Nov 2;59(45):19857-19861. doi: 10.1002/anie.202007423. Epub 2020 Sep 15.

Abstract

Polyethylene terephthalate (PET) is selectively depolymerized by a carbon-supported single-site molybdenum-dioxo catalyst to terephthalic acid (PTA) and ethylene. The solventless reactions are most efficient under 1 atmosphere of H2 . The catalyst exhibits high stability and can be recycled multiple times without loss of activity. Waste beverage bottle PET or a PET + polypropylene (PP) mixture (simulating the bottle + cap) proceeds at 260 °C with complete PET deconstruction and quantitative PTA isolation. Mechanistic studies with a model diester, 1,2-ethanediol dibenzoate, suggest the reaction proceeds by initial retro-hydroalkoxylation/β-C-O scission and subsequent hydrogenolysis of the vinyl benzoate intermediate.

Keywords: heterogenous catalysis; hydrogenolysis; molybdenum; polymers; reaction mechanisms.