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Carbon-silica dual-phase filler (CSDPF)/natural rubber (NR) vulcanizate was prepared by mechanical blending, followed by a hot-press vulcanization. The dispersion of CSDPF in the NR matrix and the effects of CSDPF on the filler-rubber interaction and structure of the rubber network were studied. Scanning electron microscope results showed that CSDPF dispersed uniformly; however, there were some aggregates of CSDPF when loading too many fillers. With an increase in CSDPF, the interaction between CSDPF and NR chains increases, which was detected by bound rubber in the CSDPF/NR compound. The spectra of solid-state nuclear magnetic resonance revealed that CSDPF could promote the formation of poly-sulfidic crosslink in the rubber vulcanization network. Further, the molecular chain movement ability of vulcanizates decreases according to the spin-spin relaxation of 1 H nuclei in CSDPF/NR compounds. The crosslink density of vulcanizate increases, while the chemical crosslink and physical crosslink in the vulcanization network also increase according to the tube model.

The Effects of Carbon–Silica Dual-Phase Filler on the Crosslink Structure of Natural Rubber