Trailblazing 3D MOFs Featuring 1,2,4‐Dinitrimino Triazole: Redefining Energetic Materials and Iodine Encapsulation

Abstract The quest for high‐performance energetic materials for defense and aerospace has intensified, focusing on balancing energy output and safety. This study presents the synthesis of 3D energetic metal‐organic frameworks (EMOFs) [Na 3 (DNT)(H 2 O)] n ( Na‐MOF ), [K 2 (DNT) 2 (H 2 O)] n ( K‐MOF ), and [Cs 2 (DNT)] n ( Cs‐MOF ) using 1,2,4‐dinitrimino triazole (DNT) through a hydrothermal process. The synthesized EMOFs are characterized using infrared spectroscopy, powder X‐ray diffraction, scanning electron microscopy (SEM), elemental analysis, and thermogravimetric analysis and differential scanning calorimetry, and structures confirmed via single‐crystal X‐ray diffraction, revealing 3D frameworks with crystal densities of 2.15, 2.16, and 2.86 g cm −3 , respectively. Among them, Na‐MOF exhibits excellent detonation performance (VOD = 8900 m s −1 , DP = 26.21 GPa), high thermal stability (T d = 369 °C), and insensitivity to impact and friction (IS = 40 J, FS = 360 N). K‐MOF displays balanced energetic and mechanical properties, while Cs‐MOF , though moderate in energetic performance, shows significant potential in pyrotechnic applications, producing a bright red flame. Intermolecular interactions are analyzed through Hirshfeld surface, 2D fingerprint, and SEM analyses, enhancing the understanding of particle size and morphology. Na‐MOF also demonstrates high iodine encapsulation capacity, positioning it as a potential replacement for traditional materials like RDX and heat‐resistant explosives such as HNS, with comparability to PYX.