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Catalytic stability is the prerequisite for the catalyst to achieve high catalytic efficiency. This study finds a new path that Prussian Blue (PB) ultrathin nanosheet assembly material (PB‐NSa) is designed and used to reach efficient catalysis through continuous interaction with ammonium perchlorate (AP, component to be catalyzed). Based on the strong oxidation environment provided by AP, the decomposition of PB occurs in advance, the product Fe2O3 accelerates the decomposition of AP that can release a large amount of gas, then reacts on Fe2O3 and disperses it near the undecomposed AP, finally realizing continuous and efficient catalysis. The results show that under the catalysis of PB‐N, "deactivation" stage of AP thermal decomposition disappears, showing two consecutive exothermic stages, high temperature decomposition peak of AP is reduced to 341.1 °C, the reduction range is 73.1 °C. Combining kinetic calculation and TG‐IR test, it is found that PB‐NSa can keep excellent catalytic stability, which depends on its special structure and interaction with AP. This research provides a design idea for the material to achieve catalytic stability, which will greatly promote its rapid industrialization. [ABSTRACT FROM AUTHOR]

Burning rate of solid propellants can be effectively improved by adding catalysts and using smaller size ammonium perchlorate (AP). Although few reports, the exploration of changing the size of AP primary particles by catalysts is of great significance for improving combustion performance. Here, taking Co‐bipy as an example, the potential advantages of such materials as AP decomposition catalysts are reported. Due to the existence of NO3− combined with oxygen rich environment provided by AP, the structural self‐transformation from micronrods to nanoparticles can be quickly realized during the heating process. More importantly, when Co‐bipy decomposes, it can play the role of "scalpel" and in situ cut AP particles. Results show that high‐temperature decomposition of Co‐bipy/AP occurs at 305.8 °C, which is 137.5 °C lower than that of pure AP. Catalytic mechanism is discussed by in situ IR and TG‐IR, CoO can effectively increase the content of reactive oxygen species and weaken the N–H bond, realizing the rapid oxidation of NH3. Eventually, the behavior of Co‐bipy cutting AP particles is tested. This interesting catalyst structure self‐transformation behavior can not only realize the influence on AP, but also perform a positive function in the combustion process of solid propellants, such as opening the adhesive AP interface. [ABSTRACT FROM AUTHOR]