Synergistic Computational-Experimental Discovery of a Zwitterionic Fused-Ring High-Energy-Density Material with...

The relentless pursuit of high-energy-density materials (HEDMs) is fundamentally constrained by the inherent trade-off between energy output and molecular stability. Nitrogen-rich fused-ring scaffolds have emerged as a privileged platform to navigate this challenge, yet the systematic exploration of their chemical space and the rational design of derivatives that simultaneously achieve high energy, low sensitivity, and favorable physicochemical properties remain elusive. Herein, we report a synergistic computational-experimental strategy that integrates high-throughput screening with rational molecular design to discover a new class of [5,6,5] fused-ring energetic zwitterions. Starting from a combinatorially enumerated library of nearly ten million [5,6,5] fused-ring structures, we employed a validated performance-prediction modelincorporating machine learning and quantum chemical calculationsto iteratively screen for candidates with an optimal balance of high density, low impact sensitivity, and high thermal stability. This process identified a unique structural motif that merges the stabilizing conjugation of a planar, nitrogen-rich fused framework with the dense-packing advantages of a zwitterionic architecture, effectively addressing the long-standing acidity issue associated with traditional NTO-based materials. This guided approach culminated in the successful synthesis of a lead compound, TYX-7. Critically, TYX-7 exhibits a measured density of 1.95 g/cm³, a detonation velocity of 9.113 km/s, a detonation pressure of 35.4 GPaperformance metrics on par with HMXalong with low mechanical sensitivity (IS > 40 J, FS > 360 N) while retaining the low sensitivity characteristic of NTO. Beyond its impressive energetic performance, TYX-7 demonstrates exceptionally low ignition delay (130.0 ms at 70 W/cm²), sustained and stable combustion over extended durations, and remarkably clean burning with minimal smoke generation, underscoring its promise for practical applications. Its measured pK _a of 5.99 signifies a remarkable shift toward neutrality, overcoming the corrosive drawback of its predecessor. This work not only delivers a promising new HEDM candidate but also establishes a robust, transferable paradigm for the accelerated discovery and design of next-generation energetic materials.