A styrene-butadiene rubber having a gradient crosslink density in the thickness direction was simply prepared by vulcanizing under a temperature gradient to study its mechanical properties and swelling behavior. The graded rubber exhibited considerable strain recovery after stress removal despite having a low crosslinked part. Notably, the graded rubber also manifested greater hysteresis loss during cyclic test compared to a homogeneously crosslinked rubber, even though they had similar initial moduli. Furthermore, anomalous swelling behavior was observed in the graded rubber. The graded rubber exhibited shape transformation upon swelling. The mechanism was thoroughly explained using gel swelling theory under constraints. This must be a common phenomenon in graded rubbers with a crosslink gradient in the thickness direction. This comprehensive research provides a novel approach for material design with tailored properties and promising applications for this potential material.
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