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Ionizing Radiation
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Polymer radicals can also be produced by the irradiation of a polymer monomer mixture with ionizing radiation. Thus, the interaction of ionizing radiation with polyethylene styrene produces radical centers on polyethylene, and these initiate graft polymerization of styrene to produce poly(ethylene-graft-styrene) [Rabie and Odian, 1977]. Most radiation graft polymerizations are carried out as heterogeneous reactions. The polymer is swollen by monomer but does not dissolve in the monomer. (For semicrystalline polymers, swelling and grafting take place only in the amorphous regions.) The typical reaction system involves equilibration of polymer with monomer followed by irradiation of the
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+ H CH2CH (CH2CH )n
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9-51 9-52
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monomer-swollen polymer while immersed in excess monomer. Whether graft polymerization occurs uniformly throughout the volume of the polymer or mainly at its surfaces depends on the rate of monomer diffusion into the polymer relative to the grafting rate [Cardona et al., 2002; Imre and Odian, 1979; Odian et al., 1980]. For reaction systems with slow diffusion rates and/or fast grafting rates, the overall process becomes diffusion-controlled, with the observed grafting rate limited by the rate of diffusion of monomer into polymer. Anomolous kinetic behavior is observed under these reaction conditions; for example, the reaction rate becomes greater than rst-order in monomer, less than half-order in initiation rate, and inversely dependent on the thickness of the polymer sample. Most graft polymerizations, irrespective of the initiation process, yield mixtures of the graft copolymer, ungrafted backbone polymer, and homopolymer of the monomer. The relative amounts of the three species depend on the monomer polymer combination and the initiation process. For initiation by chain transfer, the ef ciency of the grafting reaction relative to homopolymerization is dependent on the tendency of a propagating radical to transfer to polymer compared to propagation. A consideration of CP values (Sec. 3-6d) indicates that the extent of homopolymerization will be very signi cant during graft polymerization. The grafting ef ciency of the irradiation process is often discussed in terms of the relative extents of radical formation in the polymer and monomer. Combinations of a polymer such as polyethylene (relatively susceptible to radiolytic bond cleavage) and a monomer such as styrene (relatively resistant to radiolytic bond cleavage) are generally considered to involve minimal homopolymerization relative to graft polymerization. However, this conclusion is somewhat naive as it assumes that hydrogen atoms formed in the radiolytic initiation step (Eq. 9-51) will mostly form molecular hydrogen. This is unlikely in the presence of monomer, which should scavenge at least some of the hydrogen radicals. The extent of homopolymerization equals that of graft polymerization if all hydrogen radicals initiate homopolymerization [Machi and Silverman, 1968]. The range of radiation grafting systems studied is enormous; almost all of the more common monomers such as styrene, methyl methacrylate, vinyl chloride, and acrylonitrile have been grafted to most of the commercially available addition and condensation polymers [Chapiro, 1962; Wilson, 1974]. One commercial application of radiation processing is the curing of wood impregnated with monomers for high-performance commercial ooring.
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The product involves a combination of homopolymerization and graft polymerization of a monomer such as methyl methacrylate to wood. Graft polymerization can also be achieved by irradiation with ultraviolet radiation, often in the presence of a photosensitizer such as benzophenone or benzoin [Guthrie et al., 1979; Tazuke and Kimura, 1978]. Photolytic grafting is similar to radiation grafting, except that the depth of penetration by UV is far less than by ionizing radiation. 9-9a-4 Redox Initiation
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Redox initiation is often an ef cient method for graft polymerization. Hydroxyl-containing polymers such as cellulose and poly(vinyl alcohol) undergo redox reaction with ceric ion or other oxidizing agents to form polymer radicals capable of initiating polymerization
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