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reactivity of almost all monomers in radical polymerization (Sec. 3-1b). However, only certain comonomer pairs undergo cationic or anionic copolymerization. For example, both styrene acrylonitrile and styrene ethyl vinyl ether undergo radical copolymerization, but there is great selectivity in ionic copolymerizations. Styrene acrylonitrile undergoes anionic polymerization, but not cationic copolymerization. Styrene ethyl vinyl ether undergoes cationic copolymerization, but not anionic copolymerization. For any speci c type of initiation (i.e., radical, cationic, or anionic) the monomer reactivity ratios and therefore the copolymer composition equation are independent of many reaction parameters. Since termination and initiation rate constants are not involved, the copolymer composition is independent of differences in the rates of initiation and termination or of the absence or presence of inhibitors or chain-transfer agents. Under a wide range of conditions the copolymer composition is independent of the degree of polymerization. The only limitation on this generalization is that the copolymer be a high polymer. Further, the particular initiation system used in a radical copolymerization has no effect on copolymer composition. The same copolymer composition is obtained irrespective of whether initiation occurs by the thermal homolysis of initiators such as AIBN or peroxides, redox, photolysis, or radiolysis. Solvent effects on copolymer composition are found in some radical copolymerizations (Sec. 6-3a). Ionic copolymerizations usually show signi cant effects of solvent as well as counterion on copolymer composition (Sec. 6-4). The monomer reactivity ratios and copolymer compositions in living copolymerizations are generally the same as those in the corresponding nonliving systems. However, Matyjaszewski [2002] has described reaction conditions that result in deviations in copolymer compositions for some living systems. The differences arise not from differences in monomer reactivity ratios, but from differences in the consumption of the two monomers. The effect is observed in living systems where there is a recycling equilibrium (activation and deactivation) between active and dormant species. This applies to radical systems such as ATRP, NMP, and RAFT, as well as many ionic systems, which involve an activation and deactivation equilibrium. For a copolymerization, there is a separate activation deactivation equili* * brium for each of two different propagating species (M1 and M2 ). Deviations are possible only when two conditions exist. First, the two propagating species must have different activation and/or deactivation rate constants. Second, the homopropagation rate constant for each propagating species must be different from its cross-propagation rate constant; in other words, both r1 and r2 are not one. Under these conditions, one of the monomers is consumed faster than in the corresponding nonliving system. The comonomer feed and, therefore, the copolymer composition, change with conversion differently from the nonliving system. The deviations in copolymer composition are greater when homopropagation is faster than cross-propagation (r1 , r2 > 1) than when cross-propagation is faster than homopropagation (r1 , r2 < 1). 6-2d Types of Copolymerization Behavior
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Different types of copolymerization behavior are observed depending on the values of the monomer reactivity ratios. Copolymerizations can be classi ed into three types based on whether the product of the two monomer reactivity ratios r1 r2 is unity, less than unity, or greater than unity. 6-2d-1 Ideal Copolymerization: r1 r2 1
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A copolymerization is termed ideal when the r1 r2 product is unity. Ideal copolymerization * * occurs when the two types of propagating species M1 and M2 show the same preference for
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adding one or the other of the two monomers. Under these conditions
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and the relative rates of incorporation of the two monomers into the copolymer are independent of the identity of the unit at the end of the propagating species. For an ideal copolymerization Eq. 6-28 is combined with Eq. 6-12 or 6-15 to yield the copolymerization equation as
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