Unveiling the Role of Curvature in Carbon for Improved Energy Release of Ammonium Perchlorate

ABSTRACT The catalytic role of carbon curvature in the thermal decomposition of ammonium perchlorate (AP) remains largely unexplored. To address this gap, this study employs machine learning and density functional theory to expedite the screening of curved carbon materials for enhanced catalytic energy release from AP. High‐curvature carbon nanotubes (H‐CNTs) exhibit superior performance by tuning the carbon p ‐band center, which strengthens the adsorption of key intermediates of AP decomposition (e.g., HClO 4 ). H‐CNT lowers the AP decomposition temperature by 103.5°C and dramatically amplifies heat release by a factor of 6.6 (increasing from 250.7 to 1898.5 J g −1 ). In addition, enhanced safety, increased maximum output pressure (from 5.9 to 135.3 kPa) and a markedly improved combustion effect (ignition in just 2 ms) are also observed with high‐curvature CNTs. These findings underscore curvature as a critical design parameter and provide a geometry‐electronic‐activity framework for developing efficient catalysts in energetic materials.