Interfacial Electronic Reconstruction and Thermal Boundary Layer Compression Synergy in Three-Dimensional Coral-like...

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.