High-energy-density photosensitive pyrotechnics with good thermal stability have been in increasing demand in recent years. In this paper, graphene oxide (GO)-intercalated energetic coordination polymers (ECPs) are prepared with improved thermostability but great photosensitivity by using high nitrogen compounds azotetrazole (AT) and 5,5′-bistetrazole-1,1′diolate dehydrate (BTO) as ligands. The decomposition activation energy (E a ) of Cu-AT has been increased from 135.7 to 151.9 kJ• mol −1 after intercalating 5 wt% GO, and in the meantime, the exothermic peak temperature (T p ) was increased by 12.6 °C. However, the decomposition E a of Cu-BTO decreased under the effect of the same amount of GO with little effect on T p . This confirms that GO has stabilization effects on the Cu-AT crystal, whereas the catalytic effects on Cu-BTO would dominate after dehydration with its crystal lattice collapse. Also, when the content of GO was 3%, the resultant GO 0.03 -Cu-AT exhibits a higher density (2.88 g•cm −3 ) and good thermostability (T p = 293.7 °C). This ECP shows excellent low-energy laser ignition performance, which can be ignited with an energy of less than 1 mJ at a wavelength of 976 nm. Low-energy laser initiation is considered to be a safer but more reliable method than the traditional electrical-based ones.
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