Disorder Driven Triphenylamine Based Monolithic Covalent Organic Framework for the Efficient Removal of Toxic Oxo‐Anions From Water

Abstract Covalent Organic Frameworks (COFs) have garnered significant attention for environmental remediation due to their ordered porosity, high surface area, and exceptional contaminant removal properties. However, the synthesis of pure‐phase monolithic COFs and their application in water remediation is still in the infancy stage. Herein, an industrial‐friendly and eco‐friendly ball‐mill‐assisted in‐situ gas forming approach is developed for the synthesis of pure phase monolithic COF, named BPTP Foam, that efficiently removes the toxic oxoanions from water. This approach induces a hierarchical porous structure, providing high adsorption capacities of 961.54 mg g −1 for MnO₄⁻ and 448.09 mg g −1 for CrO₄ 2 ⁻, with rapid removal times of 1 and 3 min, respectively. Notably, the adsorption capacity for MnO₄⁻ is the highest among all porous materials reported to date. Density Functional Theory (DFT) and adsorption studies reveal that strong non‐covalent interactions between the peripheral oxygen atoms of metal anions and the triphenylamine moieties within the framework contribute to enhancing removal kinetics. The simplicity and scalability of the synthesis method, combined with the high performance of BPTP Foam, make it a promising candidate for large‐scale environmental remediation applications.