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It is demonstrated that the often observed broadness of the molecular weightdistribution obtained from latex particles synthesized by means ofsurfactant-free emulsion polymerization results from the multistage kinetics.The initial stage of the polymerization, by which the primary particles areformed, is of the 01-kind which means that it can be assumed that the particlesare so small that at any moment of time there is no more than one radical chainper particle. After the aggregation of primary particles into secondaryparticles, the so called coagulative nucleation step, the polymerizationkinetics in the subsequently coalesced secondary particles is of thepseudo-bulk kind which means that there are so many radicals in the particlesthat the polymerization process proceeds as in bulk. The important consequenceis that the molecular weight of the 01-process is about one order of magnitudelarger than that of the pseudo-bulk process. Hence, each of thesepolymerization modes and the aggregation stage in-between leave their traces inthe molecular weight distribution as is shown by experiments aimed atprolonging the initial formation kinetics. Bimodal molecular weightdistributions are found both for ionic and non-ionic initiators.

Bimodal molecular mass distribution in surfactant-free emulsion polymerization as a consequence of coagulative nucleation