Catalytic oxidation upcycling of polyethylene terephthalate to commodity carboxylic acids

This is the authors' abstract. We don't add key points for this paper.

Catalytic upcycling of polyethylene terephthalate (PET) into high-value oxygenated products is a fascinating process, yet it remains challenging. Here, we present a one-step tandem strategy to realize the thermal catalytic oxidation upcycling of PET to terephthalic acid (TPA) and high-value glycolic acid (GA) instead of ethylene glycol (EG). By using the Au/NiO with rich oxygen vacancies as catalyst, we successfully accelerate the hydrolysis of PET, accompanied by obtaining 99% TPA yield and 87.6% GA yield. The results reveal that the oxygen vacancies in NiO (NiO-Ov) support tend to adsorb hydrolysis product TPA, preferentially ensuring the strong adsorption of EG at the Au-NiO interface. Moreover, during the EG oxidation process, the Au-NiO interface, composed of two types of structures, quasi "AuNi alloy" and NiO-Ov, simultaneously promote the C-H bond activation, where Ni in "AuNi alloy" exhibits an oxytropism effect to anchor the C = O bond of the intermediate, while the residual O in NiO-Ov pillages the H in the C-H bond. Such Au/NiO catalyst is further extended to promote the thermal catalytic oxidation upcycling of other polyethylene glycol esters to GA with excellent catalytic performance.