In an effort to support the recycling of rubbery polymers and composit
es, H-1 NMR relaxation and pulsed-gradient spin echo diffusion measure
ments have been performed on virgin and unfilled vulcanized strene-but
adiene rubber (SBR), and networks after various extents of devulcaniza
tion using an ultrasound technique. The NMR methods recognize unentang
led light molecules (e.g. sol), but do not distinguish between unattac
hed entangled large molecules and chemical network segments. Devulcani
zation generates additional soi with a wide mass distribution, thus in
creasing both sol and gel mobility, but decreasing sol mean diffusivit
y. The latter effect is accounted for by the increasing mean sol molec
ular mass but also by the increasing glass transition temperature, whi
ch is related to main-chain stiffening seen in our earlier C-13 NMR ex
periments. In addition to improving the molecular-level understanding
of devulcanization, this study provides guidance for the optimization
of the devulcanization parameters.