Revealing the Effect of Copper Single‐Atom Catalyst for Improved Energy Release of Ammonium Perchlorate

ABSTRACT Catalyzing ammonium perchlorate (AP) thermal decomposition is essential for improving the energy release of composite solid propellants. Single‐atom catalysts (SACs) show great potential in AP catalysis, but systematic research on their regulation of AP decomposition and propellant combustion remains insufficient. Herein, four carbon black‐supported transition metal single‐atom catalysts (M‐SACs, M = Fe, Co, Ni, Cu) were prepared via a coordination adsorption‐pyrolysis strategy, and their atomic dispersion and coordination structure were systematically characterized. Thermal tests demonstrate that Cu‐SAC delivers the best catalytic performance, reducing AP's high‐temperature decomposition peak by 103.6°C, increasing heat release by 4.1 times, and lowering activation energy by 96.3 kJ/mol. Molecular dynamics simulations confirm that Cu‐N active sites strongly adsorb key intermediates (NH 3 and HClO) and weakly bind final products, providing a thermodynamic basis for its superior catalytic activity. In AP‐based propellants, Cu‐SAC increases burning rate by 25.6% and shortens ignition delay by 23.1%, while effectively suppressing molten aluminum agglomeration and reducing condensed combustion product size by 61%. This work establishes the multi‐scale structure‐activity relationship of Cu‐N coordination, offering a new route for the design of high‐performance propellant combustion catalysts.