An Oxygen-Defect-Induced Unsaturated Coordination Strategy Boosts High-Selective PET Upcycling via Suppressing Oxygen Evolution.

Authors

Xingye Lu, Jia Song, Yuhao Guo, Congcong Liang, Yuanyuan Liu, Zeyan Wang, Hefeng Cheng, Zhaoke Zheng, Yaqiang Wu, Baibiao Huang, Peng Wang

Published in

Angewandte Chemie (International ed. in English). Pages e3451583. Jul 03, 2026. Epub Jul 03, 2026.

Abstract

Electrochemical upcycling of polyethylene terephthalate (PET) plastics coupled with hydrogen production offers a sustainable pathway for carbon reutilization and energy sustainability. However, PET-derived ethylene glycol electro-oxidation reaction (EGOR) in alkaline conditions inevitably competes with oxygen evolution reaction (OER) due to enhancing OH^- utilization for OER under industrially relevant high-current conditions, reducing electrolysis efficiency and degrading catalyst stability. In this study, we precisely regulate oxygen-defect concentration to construct an unsaturated CoFeO_x(OH)_y/CFP catalyst, achieving 93% ± 2% Faradaic efficiency (FE) for formic acid and over 700 h of stability. In situ characterizations and theoretical calculations show that oxygen defects tune the surface electronic structure and promote the timely consumption of electrochemically generated MO_x(OH)_y species by EG preventing the excessive accumulation of high-valence species and suppressing OH^- evolution into oxygenated OER intermediates. By balancing MO_x(OH)_y formation with its spontaneous reaction with EG, OH^- utilization toward EGOR is enhanced, enabling efficient OER suppression at high anodic potentials. Furthermore, a large-scale three-cell electrolyzer (300 cm² per piece) achieves 17.4 A at 3 V with nearly 100% FE for hydrogen production, reducing energy consumption by > 21.05% compared with overall water splitting. This work provides mechanistic insights and a practical strategy for industrial PET upcycling integrated with low-energy hydrogen production.

PMID:
42397802
Bibliographic data and abstract were imported from PubMed on 04 Jul 2026.

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