Abstract
A computer simulation model of free radical crossi inking polymerization is used to probe inhomogeneity in gelation in context to recent experimental speculations.In this chapter, a computer simulation model of free radical cross-linking polymerization is presented, which is used to probe inhomogeneity in gelation in context to recent experimental speculations. The extent of inhomogeneity in amorphous polymeric materials is a difficult issue both experimentally and theoretically. While linear polymers are now believed to be homogeneous, there are strong indications that many cross-linked polymers are not. It has been observed that the relative number of pendant double bonds (PDBs), that is, unreacted vinyl groups on polymer segments in monovinyl/divinyl polymerization per divinyl repeat unit drops off very fast at low conversion and then decreases only slowly as a function of weight conversion. The sharp drop points to the formation of highly intramolecularly cross-linked macromolecules. The slow decrease is interpreted as the shielding of PDBs within macromolecular structures from further reaction by fully reacted polymer. The chapter focuses on this conversion dependence of the number of PDBs.
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