Co-vulcanization of natural rubber (NR) and high-moduli Eucommia ulmoides gum (EUG) is promising while the reduction in crystallinity of crosslinked EUG is adverse for developing high-performance materials. Proposed herein is a novel method to prepare high-strength and high-stretchability NR/EUG vulcanizates with rapid vulcanization of EUG into slightly crosslinked particles, followed by further vulcanization of NR to form crosslinked matrix network. Deep eutectic solvents (DESs) are employed to facilitate the vulcanization of EUG during its blending with NR. The two-step vulcanization results in vulcanizates exhibiting superior mechanical properties under shear, tensile, and compressive conditions, significantly exceeding those of vulcanizates prepared by traditional processing methods. The reinforcement mechanism is elucidated by controlling thermomechanical coupling conditions and is supported by comprehensive structural characterizations. It is suggested that the EUG crystalline regions, maintained through the special processing method, work in conjunction with the stress-induced crystallization of the matrix to enhance the vulcanizates, nearly doubling the deformation stress at 800% strain. The crystalline regions can mediate the deformation stress during shear and compression and weaken nonlinear rheological behavior. The established structure-performance relationship is guidable for preparing high-performance NR/EUG blend vulcanizates.
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