Plasma-induced fluorine recycling from perfluoroalkyl acid into active MOF catalysts: Unlocking lattice oxygen for enhanced electrocatalysis

Underwater plasma enables one-step PFAA degradation and F-doped CoFe 0.5 BDC synthesis. • F-doping optimizes electron transfer and enhance adsorption of *OH intermediates. • F-doping unlocks lattice oxygen activation at the Fe/Co dual sites. • The LOM-driven OER pathway significantly lowers the reaction barrier. Electrocatalytic water splitting faces efficiency challenges due to sluggish oxygen evolution reaction (OER) kinetics. Here, we develop an underwater spark plasma discharge strategy to simultaneously degrade perfluoroalkyl acids (PFAAs) and synthesize F-doped CoFe 0.5 BDC electrocatalysts using recovered fluorine. The resulting F 7 -CoFe 0.5 BDC (derived from heptafluorobutyric acid) exhibits exceptional OER performance in alkaline media, achieving a low overpotential of 271 mV at 10 mA cm −2 with robust stability. In-situ characterization and density functional theory (DFT) calculations reveal that F-doping activates the lattice oxygen mechanism (LOM) by optimizing electron transfer and enhancing adsorption of *OH intermediates at Fe/Co dual sites. This work integrates pollutant degradation with circular catalyst fabrication, establishing a sustainable paradigm for designing high-performance OER electrocatalysts via lattice oxygen activation. A sustainable “pollutant-to-catalyst” upcycling strategy is developed via an underwater spark plasma method, which enables simultaneous perfluorinated pollutant degradation and the in-situ synthesis of F-doped CoFe-BDC. The incorporated F atoms activate the lattice oxygen mechanism on adjacent Fe/Co dual sites, significantly lowering the OER energy barrier. This work provides a green, generalizable pathway to design high-performance electrocatalysts from environmental waste streams. Download: Download high-res image (141KB) Download: Download full-size image