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An Oxygen-Defect-Induced Unsaturated Coordination Strategy Boosts High-Selective PET Upcycling via Suppressing Oxygen
Xingye Lu1, Jia Song1, Yuhao Guo2
1State Key Laboratory of Crystal Materials, Shandong University, Jinan, China.
Angewandte Chemie (International Ed. in English)
|July 3, 2026
Summary
This study enhances polyethylene terephthalate (PET) upcycling for sustainable hydrogen production by creating a novel catalyst. This catalyst suppresses competing reactions, improving efficiency and stability for carbon reuse.
Area of Science:
- Electrochemistry
- Materials Science
- Sustainable Chemistry
Background:
- Electrochemical upcycling of polyethylene terephthalate (PET) plastics combined with hydrogen production presents a sustainable route for carbon reuse and energy sustainability.
- The electro-oxidation reaction of PET-derived ethylene glycol (EGOR) in alkaline media faces competition from the oxygen evolution reaction (OER), especially under high-current conditions, reducing efficiency and catalyst stability.
Purpose of the Study:
- To develop a catalyst that precisely regulates oxygen-defect concentration for efficient EGOR and suppressed OER.
- To investigate the mechanistic insights of oxygen defects in tuning catalyst performance for PET upcycling and hydrogen production.
Main Methods:
- Fabrication of an unsaturated cobalt-iron oxide/hydroxide catalyst (CoFeOx(OH)y/CFP) with controlled oxygen defects.
- In situ characterizations and theoretical calculations to understand the role of oxygen defects in reaction pathways.
- Testing of a large-scale three-cell electrolyzer for integrated PET upcycling and hydrogen production.
Main Results:
- The engineered CoFeOx(OH)y/CFP catalyst achieved 93% ± 2% Faradaic efficiency for formic acid and over 700 hours of stability.
- Oxygen defects were shown to tune the electronic structure, promoting EG consumption and suppressing OER by preventing accumulation of high-valence species.
- A large-scale electrolyzer demonstrated 17.4 A at 3 V with nearly 100% Faradaic efficiency for hydrogen production, reducing energy consumption by >21.05% compared to overall water splitting.
Conclusions:
- Regulating oxygen defects in CoFeOx(OH)y/CFP catalysts is a viable strategy to enhance EGOR selectivity and suppress OER.
- The developed catalyst and integrated system offer a practical approach for industrial PET upcycling coupled with low-energy hydrogen production.
- This work provides crucial mechanistic understanding for designing advanced electrocatalysts for sustainable chemical transformations.
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