Amorphization enabled deep self-reconstruction of bimetallic metal-organic frameworks for efficient and robust oxygen...

Precise regulation of self-reconstruction in metal-organic frameworks (MOFs) presents a promising strategy for designing high-performance oxygen evolution reaction (OER) electrocatalysts. In this study, we introduce an amorphization strategy to induce profound self-reconstruction in bimetallic tetrathiafulvalene tetrabenzoate (H₄TTFTB) MOFs supported on nickel foam (NF). The optimized Co₃Fe₁-TTFTB@NF electrocatalyst exhibits remarkably low overpotentials (228 mV at 10 mA cm^-2, 267 mV at 100 mA cm^-2) and maintains stability for 200 h at 100 mA cm^-2, outperforming commercial RuO₂ and most reported MOF-based catalysts. Operando Raman spectroscopy, combined with density functional theory (DFT) calculations, reveals that Fe incorporation reduces the oxygen vacancy formation energy and promotes amorphization, enabling profound reconstruction into (Co₃Fe₁)OOH. This (Co₃Fe₁)OOH phase demonstrates a low theoretical OER overpotential of 0.68 V. This work establishes amorphization engineering as a general design strategy for highly efficient and stable MOF-derived alkaline water oxidation catalysts.