The slow regression rate induced by the high pyrolysis difficulty has limited the application and development of hydroxyl-terminated polybutadiene (HTPB)-based fuels in hybrid rocket propulsion. Nickel oxide (NiO) shows the possibility of increasing the regression rate of HTPB-based fuels by catalyzing the pyrolysis process of the polymer matrix in our previous investigation; hence, this paper studies the NiO particles in the thermal decomposition and combustion of HTPB fuel grains. The DSC/TG test shows that NiO can intensely decrease the thermal stability of HTPB, and the catalytic effect of NiO is mainly reflected in the final decomposition stages of polybutadiene components. 5 wt% NiO enhances the regression rate by 19.4% and 13.7% under an oxygen mass flux of 50 kg/m2s and 150 kg/m2s, respectively. Further investigation shows that NiO particles will also cause the reduction of combustion heat and the agglomeration at the regressing surface while catalyzing the pyrolysis process, improving the thermal conductivity, and promoting the radiative heat transfer of the HTPB-based fuels; thus, more NiO additive (5 wt% < [NiO] ≤ 10 wt%) does not lead to a faster regression rate in HTPB-based fuels. This study demonstrates the catalytic effect of NiO on the polymer matrix for HTPB-based fuels, showing the attractive application prospects of this additive in HTPB-containing fuel grains.
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