The pursuit of heat-resistant energetic materials(HREMs)with thermal stability beyond 450℃ presents a significant challenge that has yet to be achieved.In this work,we develop an innovative electronic delocalization ...The pursuit of heat-resistant energetic materials(HREMs)with thermal stability beyond 450℃ presents a significant challenge that has yet to be achieved.In this work,we develop an innovative electronic delocalization strategy to design and synthesize a planar dizwitterionic diamino-bistriazolotetrazine,designated as TYX-1.The unique structural feature of TYX-1,including a nitrogen-rich fused ring system,planar conformation,and dizwitterionic configuration,combined with its hydrogen-bonded organic framework(HOF)structure,confer exceptional thermal stability(The onset temperature is 428℃,and the peak temperature is 473℃),high density(1.84 g/cm^(3)),and remarkable detonation performance(detonation velocity:8616 m/s).Furthermore,TYX-1 exhibits an impressive insensitivity(impact sensitivity>40 J;friction sensitivity>360 N),surpassing all previously reported HREMs.Theoretical calculations and single-crystal clearly indicate that the delocalizedπelectrons within the dizwitterionic bistriazolotetrazine rings and the HOF structure of TYX-1 are pivotal in ensuring its high thermal stability and high energy density.The discovery of TYX-1 marks a significant advancement in the field of HREMs and is anticipated to catalyze substantial progress in various high-temperature applications reliant on energetic materials.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.22105156,22175139,22505195,22171136,22405207 and 22302156)the China National Science Fund for Distinguished Young Scholars(Grant No.22325504)。
文摘The pursuit of heat-resistant energetic materials(HREMs)with thermal stability beyond 450℃ presents a significant challenge that has yet to be achieved.In this work,we develop an innovative electronic delocalization strategy to design and synthesize a planar dizwitterionic diamino-bistriazolotetrazine,designated as TYX-1.The unique structural feature of TYX-1,including a nitrogen-rich fused ring system,planar conformation,and dizwitterionic configuration,combined with its hydrogen-bonded organic framework(HOF)structure,confer exceptional thermal stability(The onset temperature is 428℃,and the peak temperature is 473℃),high density(1.84 g/cm^(3)),and remarkable detonation performance(detonation velocity:8616 m/s).Furthermore,TYX-1 exhibits an impressive insensitivity(impact sensitivity>40 J;friction sensitivity>360 N),surpassing all previously reported HREMs.Theoretical calculations and single-crystal clearly indicate that the delocalizedπelectrons within the dizwitterionic bistriazolotetrazine rings and the HOF structure of TYX-1 are pivotal in ensuring its high thermal stability and high energy density.The discovery of TYX-1 marks a significant advancement in the field of HREMs and is anticipated to catalyze substantial progress in various high-temperature applications reliant on energetic materials.
