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8-3 FORCES OF STEREOREGULATION IN ALKENE POLYMERIZATIONS Consider the forces that actually operate for or against stereoselectivity in a polymerization. Alkene polymerizations are considered rst. The extent of stereoselectivity in a polymerization depends on the relative rate at which an incoming monomer molecule is added with the same con guration as the preceding monomer unit compared to its rate of addition with the opposite con guration. Different forces determine the relative rates of the two modes of addition depending on whether the active end of a propagating chain is a free species (i.e., the chain end is free to rotate) or one that is coordinated (associated) with the initiator (or a component derived from the initiator). For free propagating species that are not coordinated, both modes of addition are possible. The stereoregularity of the polymer product is dependent primarily on the polymerization temperature, which determines the relative rates of the two modes of addition. The situation can be quite different when the propagating species is coordinated to the initiator. One or the other of the additions may be prevented or enhanced by the con guration of the coordination complex (usually consisting of the propagating chain end, initiator, and monomer). Under these circumstances coordination directs the mode of monomer addition in a stereoselective manner.

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Fig. 3-5 Dependence of the degree of polymerization of styrene on the polymerization rate. The effect of chain transfer to initiator is shown for t-butyl hydroperoxide (*), cumyl hydroperoxide (&). benzoyl peroxide (*), and azobisisobutyronitrile (&) at 60 C. After Baysal and Tobolsky [1952] (by permission of Wiley-Interscience, New York).

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there are a large number of relevant conditions (starting weights, minimization routine, stopping criteria, encoding of target values, numerical precision). Due to the sensitivity of the MLP model and to the fact that the surface may have multiple minima, altering any one of these will very likely lead to a different solution;

A plot of the left side of Eq. 3-111 versus [I]/[M] yields a straight line whose slope is CI . Figure 3-6 shows the plot for the t-butyl hydroperoxide polymerization of styrene [Walling and Heaton, 1965]. 3-6b-2 Monomer Transfer Constants

Using the methods described, the values of CM and CI in the benzoyl peroxide polymerization of styrene have been found to be 0.00006 and 0.055 respectively [Mayo et al., 1951]. The amount of chain transfer to monomer that occurs is negligible in this polymerization. The chain-transfer constant for benzoyl peroxide is appreciable, and chain transfer with initiator becomes increasingly important as the initiator concentration increases. These effects are shown in Fig. 3-7, where the contributions of the various sources of chain ends are indicated. The topmost plot shows the total number of polymer molecules per 105 styrene monomer units. The difference between successive plots gives the number of polymer molecules terminated by normal coupling termination, transfer to benzoyl peroxide, and transfer to styrene.

Fig. 3-6 Determination of initiator chain-transfer constants in the t-butyl hydroperoxide initiated polymerization of styrene in benzene solution at 70 C. After Walling and Heaton [1965] (by permission of American Chemical Society, Washington, DC.

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Fig. 3-7 Contribution of various sources of chain termination in the benzoyl peroxide initiated polymerization of styrene at 60 C. After Mayo et al. [1951] (by permission of American Chemical Society, Washington, DC).

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TABLE 3-4 Monomer Chain-Transfer Constantsa Monomer Acrylamide Acrylonitrile Ethylene Methyl acrylate Methyl methacrylate Styrene Vinyl acetate Vinyl chloride

All CM are for 60 C except where otherwise noted. Value at 25 C. c Data from Braks and Huang [1978]; all other data from Brandrup et al. [1999].

The monomer chain-transfer constants are generally small for most monomers in the range 10 5 to 10 4 (Table 3-4). Chain transfer to monomer places the upper limit to the polymer molecular weight that can be obtained, assuming the absence of all other transfer reactions. Transfer to monomer does not, however, prevent the synthesis of polymers of suf ciently high molecular weight to be of practical importance. CM is generally low because the reaction

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