AbstractThe self‐step growth polymerization of RAfmonomers in homogeneous, continuous flow stirred tank reactors (HCSTRs) is simulated under conditions of periodic feed concentration (with frequency ω and amplitude α). By having periodic operation, the polydispersity index of the polymer is found to increase by about 35 over the values at steady state. Periodic operation of HCSTRs is found to lead to gelation only for certain values of the frequency and the dimensionless residence time τ*. Gelling envelopes have been obtained to give conditions under which HCSTRs should be operated. These envelopes can be described in terms of two critical dimensionless residence times, τ c,1*and τ c,2*such that nongelling operation is always ensured when τ*τ c,2*, periodic operation always leads to gelation, and HCSTRs cannot be used. For τ c,1*<τ*<τ c,2*, the gelling behavior is found to depend on the functionalityf, amplitude α, and the dimen
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