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• There graphene-based transition metal coordination polymers have been evaluated as the energetic catalysts in Al-based composites. • These catalysts are well doped in the PVDF/AP matrix as the oxidizer shell of Al-based composites prepared by a spray drying method. • The high energy level but low burn rate has been achieved for the Al@PVDF/AP in presence of these graphene-based catalysts. In this paper, energetic combustion catalysts doped core–shell Al@PVDF/AP composites have been fabricated via a spray-drying method, where three kinds of graphene-based energetic coordination polymers (GECPs, GO-CHZ-Co, GO-CHZ-Ni and GO-CHZ-Cu) are employed. These composites have been characterized comprehensively in terms of morphologies, thermal decomposition behaviors, energy density, combustion performances and condensed combustion products (CCPs). The results show that the GO-CHZ-Co and GO-CHZ-Cu could increases the heat of explosion for Al@PVDF/AP composites from 6885.2 J·g−1 to 7491.0 J·g−1 and 7390.1 J·g−1, respectively, which are 8.8 % and 7.3 % higher than the blank reference samples. Moreover, the burn rates for these composites decrease when GO-CHZ-Co or GO-CHZ-Ni is included, indicating that these composites are promising candidates with improved energy density even unusually with decreased burn rates. [ABSTRACT FROM AUTHOR]

• ECs can enhance the combustion of Si/Ta. • Core-shell structure has some advantages compared with traditional mechanical mixing preparation method. • The reaction mechanism for ECs enhanced Si/Ta combustion was summarized. • Heat release efficiency of the composites could be well tuned by using different content and type of the ECs. This paper reports a group of new energetic materials (EMs) based on Si/Ta coated with recently developed high energetic composites (ECs), such as AP/NC and PVDF/CL-20. These Si/Ta-based nano-energetic composites have been prepared by both mechanical mixing method and an advanced technique of electrostatic self-assembly followed with a spray-drying process. The heat of reaction and combustion behavior of these novel Si/Ta@ECs composites, as well as the morphologies and compositions of their condensed combustion products (CCPs) have been comprehensively studied. It has been shown that the combustion efficiency of Si-Ta could be largely enhanced with the inclusion of two types of ECs. The maximum energy release was 18.39 kJ cm−3 of Si/Ta with the inclusion of ECs prepared by electrostatic self-assembly followed with spray-drying technique, which was 51.6% of the theoretical energy density of the pure Si/Ta and it is about 9.58 kJ cm−3 higher than the mechanically mixed one. It shows that the enhanced flame has improved luminosity and radiation due to increased energy content with higher reaction rate. The maximum flame-front propagation rate and the condensed phase reaction rate of Si/Ta with the addition of 10 wt% of ECs are 30.1 mm s−1 and 120.7 mg s−1, respectively. The maximum combustion wave temperature of Si/Ta-based composite was 2.4 times higher than that of pure Si/Ta without the ECs inclusion. The typical phase composition of the CCPs is composed of TaSi 2 , which is combined with a minor inclusion of Ta 2 O 5 , TaN 0.25 , TaC and Ta 5 Si 3. The two-step reaction mechanism includes the activation and propagation of the fast combustion wave of the ECs and the initiation of the post-burning reaction. [ABSTRACT FROM AUTHOR]