Wen-Long Ren, Qian Huang, Kai-Ge Guo, Cheng-Chen Zhang, Yu-Yang Zeng, Wei Zheng, De-Hao Xiong, Chen-Guang Zhu
With the increasing demand for rapid energy release in energetic systems, it is of great significance to develop novel combustion catalysts that integrate high catalytic activity with excellent heat-transfer properties. Herein, a three-dimensional coral-like CoFe2O4/LaCoO3 (CFLC) heterostructure catalyst is designed, which modulates the combustion behavior of potassium perchlorate (KP) through heterointerface electronic reconstruction and a porous framework. The optimized composition, CFLC-1, exploits strong electronic coupling between the two phases to induce a high concentration of oxygen vacancies and redox cycling of Co and Fe species, transforming the thermal decomposition of KP from a high-energy-barrier nucleation-and-growth mechanism into a low-energy-barrier phase-boundary contraction model. Consequently, the decomposition temperature is lowered by 88.6 °C, and the activation energy plummets from 378.3 to 148.3 kJ/mol. In a KP/lactose pyrotechnic system, CFLC-1 shortens the combustion time by 58.8%, compresses the effective thermal boundary layer thickness by 93%, increases the maximum spatial temperature gradient 4-fold, doubles the flame area, and raises the spectral purity from 70.4% to 88.9%. In situ infrared emission spectroscopy captures in real time a nearly 20-fold surge in the characteristic emission intensity of CO2, confirming that the gas-phase oxidation rate is accelerated at the molecular level. Mechanistic analysis reveals that the low-energy-barrier oxygen release pathway triggered by interfacial electronic reconstruction and the heat-transfer confinement effect of the three-dimensional interconnected framework are synergistic. They localize the intense exothermic reactions within a thin combustion wavefront, establishing a self-accelerating combustion cycle that enables efficient and rapid combustion of the perchlorate system. This work elucidates the synergistic mechanism between heterointerface electronic modulation and thermal boundary layer compression, offering a new strategy for the design of high efficiency combustion catalysts.