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

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,