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In this study, new highly energetic coordination polymers (ECPs) were successfully prepared by a facile chemical modification method based on functionalized graphene oxide (GO) sheets. Simple cross-linked GO layers with triaminoguanidine ligand (T) may further be bonded with crystals containing T and transition metal ions (T–M) using cobalt, zinc, silver, or iron as coordination centers, generating 2D-layered energetic hybrid ECPs crystals. Successful functionalization of the prepared ECPs was confirmed by SEM, exhibiting very small crystals (<400 nm). The thermal decomposition of the different T–M complexes, with or without GO–T, was assessed by using simultaneous differential scanning calorimetry and thermogravimetric analysis. It has been revealed that the coordination reaction of GO–T with T–M leads to the production of highly thermostable ECPs. Furthermore, the incorporation of 10% of functionalized GO has improved the thermal stability of T–M crystals. Raman spectroscopy demonstrates that both D and G bands of these new ECPs have been shifted. The different chemical bonding is also confirmed by FTIR and XRD analyses. The catalytic effect of the designed GO–T–M–T energetic composites on the decomposition of ammonium perchlorate (AP) and 1,3,5-trinitro-1,3,5-triazinane (RDX) has been investigated. The results confirmed that those ECPs have strong catalytic effect on decomposition of AP, and it may even stabilize RDX crystals before its thermolysis.

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