Atomic-scale insight into decompositions in energetic materials(EMs)is essential for harnessing energy release,which remains elusive due to both instrumental and computational limitations.Herein,we developed DeepEMs-2...Atomic-scale insight into decompositions in energetic materials(EMs)is essential for harnessing energy release,which remains elusive due to both instrumental and computational limitations.Herein,we developed DeepEMs-25,a deep-learning potential trained on diverse EMs towards accurate and efficient simulations.Applying DeepEMs‑25 to an isostructural ABX_(3)molecular perovskites series,with A-site organic cations,B-site alkali or ammonium cations,and X-site perchlorate anions,we probe the effect of cation size on reactivity.Arrhenius analysis of 100-ps trajectories reveals that increasing B‑site ionic radius simultaneously decreases X–A collision’s activation energy(enhancing reaction rates)and decreases X–A collision’s pre‑exponential factor(reducing collision frequency),producing opposing kinetic effects.Such“kinetic tug‑of‑war”explains why an intermediate‑sized cation yields maximal thermal stability by optimally balancing reactivity and collision dissipation.A similarly sized reactive cation promotes additional hydrogen-transfer pathways causing accelerating decomposition.Our findings link atomistic kinetics to macroscopic stability,informing nextgeneration EMs design.展开更多
基金funded by the National Natural Science Foundation of China(U2341287 and 22488101)Guangzhou Science and Technology Program(2024A04J6499)Fundamental Research Funds for the Central Universities,Sun Yat-sen University(23lgzy001).The funder played no role in study design,data collection,analysis,interpretation of data,or the writing of this manuscript.The computational resource was supported by the Bohrium Cloud Platform(https://bohrium.dp.tech/)and the National Supercomputing Center in Guangzhou(NSCC-GZ,Tianhe-2).M.-Y.G.thanks Chengqian Zhang and Duo Zhang for fruitful discussions.Language polishing was assisted by DeepSeek-v3 and finalized by human authors.
文摘Atomic-scale insight into decompositions in energetic materials(EMs)is essential for harnessing energy release,which remains elusive due to both instrumental and computational limitations.Herein,we developed DeepEMs-25,a deep-learning potential trained on diverse EMs towards accurate and efficient simulations.Applying DeepEMs‑25 to an isostructural ABX_(3)molecular perovskites series,with A-site organic cations,B-site alkali or ammonium cations,and X-site perchlorate anions,we probe the effect of cation size on reactivity.Arrhenius analysis of 100-ps trajectories reveals that increasing B‑site ionic radius simultaneously decreases X–A collision’s activation energy(enhancing reaction rates)and decreases X–A collision’s pre‑exponential factor(reducing collision frequency),producing opposing kinetic effects.Such“kinetic tug‑of‑war”explains why an intermediate‑sized cation yields maximal thermal stability by optimally balancing reactivity and collision dissipation.A similarly sized reactive cation promotes additional hydrogen-transfer pathways causing accelerating decomposition.Our findings link atomistic kinetics to macroscopic stability,informing nextgeneration EMs design.
