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Chain transfer is a chain-breaking reaction; it results in a decrease in the size of the propagating polymer chain. The effect of chain transfer on the polymerization rate is dependent on whether the rate of reinitiation is comparable to that of the original propagating radical. Table 3-3 shows the four main possible situations that may be encountered. Reinitiation is rapid in cases 1 and 2, and one observes no change in the polymerization rate. The same number of monomer molecules are consumed per unit time with the formation of larger numbers of smaller-sized polymer molecules. The relative decrease in X n depends on the magnitude of the transfer constant. When the transfer rate constant ktr is much larger than that for propagation (case 2) the result is a very small-sized polymer (X n 1 5) referred to as a

TABLE 3-3 Effect of Chain Transfer on Rp and X n Relative Rate Constants for Transfer, Propagation, and Reinitiation kp kp kp kp ) ktr ( ktr ) ktr ( ktr ka ka ka ka kp kp < kp < kp

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situation is much more like that which occurs in ionic copolymerizations Ring-opening copolymerizations are complicated in several ways: 1 For copolymerizations proceeding by the activated monomer mechanism (eg, cyclic ethers, lactams, N-carboxy-a-amino acid anhydrides), the actual monomers are the activated monomers The concentrations of the two activated monomers (eg, the lactam anions in anionic lactam copolymerization) may be different from the comonomer feed Calculations of monomer reactivity ratios using the feed composition will then be incorrect 2 Most ring-opening copolymerizations involve propagation depropagation equilibria, which require that experimental data be handled in the appropriate manner (Sec 6-5b), but this is usually not done The situation is more complicated in many systems because of additional equilibria between polymer and cyclic oligomer and by intermolecular chain transfer to polymer which result in reshuf ing of monomer units.

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It may be possible to avoid or minimize the reshuf ing equilibria by using mild initiators, low conversions, and highly reactive (more strained) monomers However, the situation in industrial practice usually involves conditions that result in near-complete reshuf ing of monomer units The effect of reshuf ing is evident in the anionic copolymerization of octamethylcyclotetrasiloxane (M1 ) and 1,3,5,7-tetramethyl-1,3,5,7-tetravinylcyclotetrasiloxane (M2 ) (feed ratio 9 : 1) by potassium silanolate at 130 C [Ziemelis and Saam, 1989] The initial copolymer is very rich in M2 , and this monomer is exhausted early Further reaction results not only in conversion of M1 but also redistribution of the M2 units Silicon 29 NMR shows the M2 units to be in blocks at short reaction times but statistically distributed at long reaction times Similar results have been observed in the cationic copolymerization of methyl glyoxylate and 1,3-dioxolane [Basko et al, 2000] 3.

We now look a t an MLP with a hidden layer as discussed in Section 2.1 (p. 9). Without loss of generality, we still restrict the discussion to MLPs with one output. We can readily extend these results to an MLP with more output units by simply

Counterion effects similar to those in ionic chain copolymerizations of alkenes (Secs 6-4a-2, 6-4b-2) are present Thus, copolymerizations of cyclopentene and norbornene with rhenium- and ruthenium-based initiators yield copolymers very rich in norbornene, while a more reactive (less discriminating) tungsten-based initiator yields a copolymer with comparable amounts of the two comonomers [Ivin, 1987] Monomer reactivity ratios are also sensitive to solvent and temperature Polymer conformational effects on reactivity have been observed in NCA copolymerizations where the particular polymer chain conformation, which is usually solvent-dependent, results in different interactions with each monomer [Imanishi, 1984] 4 Some ROPs proceed with the simultaneous operation of two different mechanisms, for example, NCA copolymerizations initiated by some secondary amines proceed with both the amine and activated monomer mechanisms The monomer reactivity ratios for any comonomer pair are unlikely to be the same for the two different propagations.

Any experimentally determined r values are each composites of two different r values 5 The initiator used is important for copolymerizations between monomers containing different polymerizing functional groups Basic differences in the propagating centers (oxonium ion, amide anion, carbocation, etc) for different types of monomer preclude some copolymerizations Even when two different monomer types undergo polymerization with similar propagating centers, there may not be complete compatibility in the two crossover reactions For example, oxonium ions initiate cyclic amine polymerization, but ammonium ions do not initiate cyclic ether polymerization [Kubisa, 1996] 7-12a Monomers with Same Functional Group.

Copolymerizations between pairs of cyclic esters, acetals, sul des, siloxanes, alkenes, lactams, lactones, N-carboxy-a-amino acid anhydrides, imines, and other cyclic monomers

&J considering each output unit separately. Now considering - (equation (2.6)),

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