High ablation-resistant silicone rubber exhibits a significant role in the thermal protection of space vehicles. However, its limited by the low mechanical strength in practical heat protection applications. Herein, a novel molecular network structure is proposed, which links polycarboxysilane (PCS) rigid molecules onto polydimethylsiloxane molecular chains. The use of PCS rigid chains enhances the heat resistance while reducing the material's mass ablation rate. The addition of a small quantity of PCS (0.406 mmol) increases the tensile strength of the material by 10.4 % and augmentes the static ablation residual weight by 32.8 % compared with polydimethylsiloxane. Additionally, PCS molecular modification of polydimethylsiloxane is beneficial for maintaining the stability of the char layer after oxygen acetylene ablation, making the char layer denser, and improving the interface bonding between the ceramic layer, pyrolysis layer and matrix, ultimately improving the ablation performance of polydimethylsiloxane. This work provides a new approach for development of high-performance flexible ablative materials.
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