High‐Level Disordered Metal–Organic Frameworks Synthesized by Interference‐Oriented Attachment for Electrochemical Anion Sieve

Abstract Disordered MOFs seamlessly amalgamate the robust stability and pore tunability inherent in crystalline MOFs with the advantages derived from abundant defects and active sites present in amorphous structures. This study pioneers the use of the interference‐oriented attachment (IOA) mechanism to meticulously craft the morphology and crystal growth of MIL‐101(Cr) (Cr‐MOF), resulting in the successful synthesis of a high‐level disordered Cr‐MOF boasting an enhanced array of active sites and exceptional electrochemical properties. The correlation between disordered structures and the electrochemical properties of MOFs are elucidated using the lattice distortion index and fractal dimension. The high‐level disordered MOF electrode showcases a remarkable fluoride sieving effect, outperforming conventional fluoride removal materials with a remarkable fluoride adsorption capacity of 41.04 mg_NaF g_electrodes⁻¹. First‐principles calculations, in conjunction with relevant experiments, provided further validation that the disordered structure significantly enhances the defluorination performance of the material. This study introduces a novel approach for the direct bottom‐up synthesis of high‐level disordered MOFs, showcasing their potential for applications in electrochemical water treatment.