Lingling Feng, Chenfeng Xia, Xinyao Zhang, Yan She, Huiyue Wang, Xueying Wen, Guixing Hu, Ran Niu, Jiang Gong*, Bao Yu Xia*
Mechanochemical upcycling of waste polyethylene terephthalate into hydroxyl-functionalized metal-organic framework for efficient oxygen evolution reaction
Advanced Functional Materials (2026) Accept. (IF2026 = 19.9)
Metal-organic framework (MOF) has been regarded as a promising electrocatalyst for oxygen evolution reaction (OER). However, synthesizing stable, cost-effective MOF electrocatalysts remains challenging, and the role of functionalized ligands, particularly their interplay with metal hydroxylation, remains unclear. Herein, a mechanochemistry-driven synthesis & functionalization collaborative (MSFC) strategy is developed to directly upcycle waste poly(ethylene terephthalate) (PET) into hydroxyl-functionalized MIL-88B(Fe)-OH. Firstly, in situ generated hydroxyl radicals (·OH) from homolytic cleavage of crystal water enable kilogram-scale production from recycled PET. Such MSFC strategy owns merits of organic solvent-free, atmospheric temperature and pressure, and low-cost, of which the material cost is ca. 1/34 of traditional solvothermal/hydrothermal methods. Secondly, MIL-88B(Fe)-OH exhibits low overpotential of 176 mV at 10 mA cm–2 and operates stably for 500 h at 100 mA cm–2, ranking as one of the most efficient MOF electrocatalysts. The coordination and electronic microenvironment of Fe sites are regulated via p–π interactions between –OH and the aromatic ring. Specifically, β-FeOOH forms selectively while the framework is preserved via Fe–O···H–O hydrogen bonding. Such electronic modulation optimizes oxygen intermediate adsorption and lowers the OER kinetic barrier. This work offers a scalable platform for producing low-cost, high-performance functionalized MOF electrocatalysts.