Graphical AbstractVerifiedDimensionally Programmable Covalent Organic Frameworks via Reversible Coordination-Directed Clip-off Strategy and Its Application in Uranium Extraction
Covalent organic frameworks (COFs) are promising adsorbents for uranium extraction from complex aqueous environments due to their tunable pore structures and customizable functionalities. However, conventional bottom-up assembly routes yield frameworks with fixed dimensionality, where internal pores and buried functional sites remain inaccessible, limiting dynamic optimization for uranium capture. This study introduces a reversible coordination-directed clip-off strategy that enables dimensional programming of COFs through silver-nitrogen coordination bonds and thiosulfate/silver ion regulators. The approach allows controlled cleavage and reconstruction of coordination bonds, dynamically exposing hidden binding sites and adapting the framework to uranium extraction requirements. While the strategy demonstrates high-efficiency uranium extraction, it faces challenges including increased material and operating costs from silver-based regulators, potential structural fatigue from repeated cleavage-reconstruction cycles, and limited validation beyond laboratory scale. The reversible dimensional programming is generalizable to other reticular frameworks such as metal-organic frameworks (MOFs), enabling stimuli-responsive smart materials, controlled-release carriers, and adaptive separation membranes. Integration with machine learning and computational screening could accelerate rational design of functional active sites. This interdisciplinary approach offers a pathway toward intelligent, dimensionally morphing materials for energy and environmental sustainability, though optimization of regulating components and structural durability is required for practical scalability.
