Catalytic oxidation upcycling of polyethylene terephthalate to commodity carboxylic acids

Qinghai Chen, Hao Yan (), Kai Zhao, Shuai Wang, Dongrui Zhang, Yaqian Li, Rong Fan, Jie Li, Xiaobo Chen, Xin Zhou, Yibin Liu, Xiang Feng (), Chen De () and Chaohe Yang
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Qinghai Chen: China University of Petroleum (East China)
Hao Yan: China University of Petroleum (East China)
Kai Zhao: China University of Petroleum (East China)
Shuai Wang: China University of Petroleum (East China)
Dongrui Zhang: China University of Petroleum (East China)
Yaqian Li: China University of Petroleum (East China)
Rong Fan: China University of Petroleum (East China)
Jie Li: China University of Petroleum (East China)
Xiaobo Chen: China University of Petroleum (East China)
Xin Zhou: Ocean University of China
Yibin Liu: China University of Petroleum (East China)
Xiang Feng: China University of Petroleum (East China)
Chen De: Norwegian University of Science and Technology
Chaohe Yang: China University of Petroleum (East China)

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract 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.

Date: 2024
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DOI: 10.1038/s41467-024-54822-w

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