摘要：SummaryPerformance-stability contradiction of high-energy-density materials (HEDMs) is a long-standing puzzle in the field of chemistry and material science. Bridging the gap that exists between detonation performance of new HEDMs and their stability remains a formidable challenge. Achieving optimal balance between the two contradictory factors is of a significant demand for deep-well oil and gas drilling, space exploration, and other civil and defense applications. Herein, supercomputers and latest quantitative computational strategies were employed and high-throughput quantum calculations were conducted for 67 reported HEDMs. Based on statistical analysis of large amounts of physico-chemical data, in-crystal interspecies interactions were identified to be the one that provokes the performance-stability contradiction of HEDMs. To design new HEDMs with both good detonation performance and high stability, the proposed systematic and comprehensive strategies must be satisfied, which could promote the development of crystal engineering of HEDMs to an era of theory-guided rational design of materials.Graphical AbstractDisplay OmittedHighlights•High-throughput quantum calculations conducted for 67 HEDMs directly on a crystal level•Main reason that provokes the performance-stability contradiction was identified•Systematic strategies for balancing performance and stability of HEDMs were proposedComputational Method in Materials Science; Density Functional Theory (DFT); Energy Materials; Materials Design
