Novel Fluorine-containing Energetic Materials: How Potential are They? A Computational Study of Detonation Performance

Abstract

Abstract High energy density materials (HEDMs) have emerged as a research focus due to their advantageous ultra-high detonation pressure and velocity. The key objective of this study is to design materials with the best performance. Density functional theory (DFT) was utilized to evaluate the geometric structure, energy properties, and sensitivities of 28 designed F-containing derivatives. The theoretical density (ρ) and heat of formation (HOF) were used to estimate the detonation velocity (D) and pressure (P) of the title compounds. Our study shows that the introduction of fluorine-containing substituents or fluorine-free substituents into the CHOFN backbone or the CHON backbone can significantly enhance the detonation performance of derivatives. Among them, derivative B1 exhibites the best overall performance, including superior density, detonation performance, and sensitivity (P = 58.89 GPa, D = 8.02 km/s, ρ = 1.93 g/cm³, and characteristic height H50 = 34.6 cm). Our molecular design strategy contributes to the development of more novel HEDMs with excellent detonation performance and stability. It also marks a significant step towards a material engineering era guided by theory-based rational design. Methods For an accurate analyze, we employed the B3LYP functional with the 6-31+G(d,p) basis set for geometry optimization and exploration of physicochemical properties of the materials. The minima with no imaginary frequencies were confirmed using harmonic vibrational frequency results at the same theory level. With the assistance of DFT calculation, the quantum properties of the materials were analyzed using the Chapman-Jouguet (C-J) thermodynamic detonation theory. Our broad analysis facilitated an extensive assessment of these properties.