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molecule reactions quickly shows that polymerizations cannot be carried out as closed systems [Allen and Patrick, 1974; Saunders and Dobinson, 1976; Zimmerman, 1988] For example, the equilibrium constants for a polyesteri cation is typically no larger than 1 10, K for a transesteri cation is in the range 01 1 and K for polyamidation is in the range 102 103 Although the equilibrium constant for a polyamidation is very high as K values go, it is still too low to allow the synthesis of high-molecular-weight polymer Further, even for what appear to be essentially irreversible polymerizations, reversal of polymerization is a potential problem if the by-product small molecule is not removed (or, alternately, the polymer is not removed) It is worth mentioning that K values reported in the literature for any speci c step polymerization often differ considerably.

Thus, K values for the polymerization of adipic acid and hexamethylene diamine range from a low of 250 to a high of 900 There are several reasons for these differences, not the least of which is the experimental dif culty in carrying out measurements on polymerizations involving highly concentrated systems (often containing only the monomers, without any solvent) at moderately high temperatures (200 300 C) Other reasons for the variation in K values are the effects of temperature and the concentration of the small molecule by-product on K Most step polymerizations are exothermic and K decreases with increasing temperature (see Sec 2-8a) The common practice of extrapolating values of K determined at certain temperatures to other temperatures can involve considerable error if H is not accurately known.

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If { O , 1) then ( t q - 2 will approach 0 in a direction perpendicular to the ) : decision hyperplane = 0. Thus, in the case where there in no hidden layer, there is a significant difference between the p1 and pc (with softmax) MLP models. This is illustrated in Figure 8.8 (which shows the IC for the logistic model) and Figure 8.4 (which shows the IC for the single layer pl model). Here it can be seen that the pf model will be more robust. This may account for the persistence in the 1 literature of the p model for classification long after it became apparent that it was an inappropriate model. Another point emerging from this section is that we might expect a model to be more robust than a P . l logistic regression model. This is considered further in p. 159.

The variation of K with the concentration of the small molecule by-product has been established in the polyamidation reaction but the quantitative effect has not been generally studied The effect may be due to a change of K with polarity of the reaction medium 2-4b Open, Driven System.

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The inescapable conclusion is that except in a minority of systems a step polymerization must be carried out as an open, driven system. That is, we must remove at least one of the products of the forward (polymerization) reaction so as to drive the equilibrium toward high molecular weights. It is usually more convenient to remove the small molecule byproduct rather than the polymer. When water is the by-product, it can be removed by a combination of temperature, reduced pressure, and purging with inert gas. Conveniently one often carries out step polymerizations at temperatures near or above the boiling point of water. This is usually done for purposes of obtaining desired reaction rates, but it has the added advantage of facilitating water removal. A small molecule by-product such as HCl can be removed in the same manner or by having a base present in the reaction system to neutralize the hydrogen chloride. Driving an equilibrium toward polymer requires considerable effort, since the water or hydrogen chloride or other small molecule must diffuse through and out of the reaction mixture. Diffusion is not so easy since the typical step polymerization system is fairly viscous at very high conversions. The polymerization can become diffusion-controlled under these conditions with the polymerization being controlled by the rate of diffusion of the small molecule by-product [Campbell et al., 1970]. The extent to which one must drive the system in the forward direction can be seen by calculating the lowering of the small molecule concentration, which is necessary to achieve a particular molecular weight. For the polyesteri cation (Eq. 2-58) one can rewrite Eq. 2-59 as

K p H2 O M 0 1 p 2 2-63

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