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In this work, syndiotactic polypropylene (sPP) as well as isotactic polypropylene (iPP) are cross‐linked to gain a shape memory effect. Both prepared PP networks exhibit maximum strains of 700%, stored strains of up to 680%, and recoveries of nearly 100%. While x‐iPP is stable for many cycles, x‐sPP ruptures after the first shape‐memory cycle. It is shown by wide‐angle X‐ray scattering (WAXS) experiments...
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