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Cationic living polymerization of C C monomers involves an equilibrium between covalent (dormant) and ionic (active) species ATRP involves reversible formation of radicals from the reaction of an alkyl halide with a metal The presence of aggregated species results in fractional-order dependencies of initiation and propagation rates on initiator and propagating species (Sec 5-3d-5) Polymerization of b-propiolactone (also called 2-oxetanone) shows some interesting features due to the high strain in the 4-membered ring [Duda, 1992; Jerome and Teyssie, 1989] Polymerization with the less nucleophilic initiators such as tertiary amines, metal carboxylates, and phosphines proceeds with ring opening at the alkyl oxygen bond instead of the acyl oxygen bond Initiation by stronger nucleophiles occurs by acyl oxygen as well as alkyl oxygen cleavage to give a mixture of carboxyl and alkoxide propagating centers.

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However, the carboxylate centers are unable to propagate by cleavage of acyl oxygen bonds while alkoxide propagating centers cleave both alkyl oxygen and acyl oxygen bonds Alkoxide propagating centers convert to carboxylates with time, and carboxylate centers constitute more than 95% of all propagating centers after only several propagations Polymerization of b-propiolactone in a highly polar solvent (DMF) in the presence of a crown ether shows the unexpected feature that ion-pair reactivity decreases more slowly with decreasing temperature compared to free-ion reactivity [Penczek et al, 2000a,b; Slomkowski, 1986] Solvation of free ions becomes so extensive at 20 C that they are less reactive than ion pairs 7-5b Cationic Polymerization.

and Wilkinson et al. (1995). Paola and Schowergerdt (1995) give a review of the application of MLP models to remotely sensed data.

Cationic polymerization of lactones is achieved with the range of initiators used for cyclic ethers (Sec. 7-2b) [Hofman et al., 1987a,b; Kricheldorf and Sumbel, 1988a,b; Kricheldorf et al., 1986, 1987a,b; Kubisa, 1996; Penczek and Slomkowski, 1989a,b]. Initiation was formerly thought to involve attack of a positive species on the endocyclic oxygen to form an

oxonium ion followed by propagation through acyl oxygen cleavage. However, polymer end-group analysis combined with trapping of propagating centers by reaction with triphenylphosphine indicates that this is not the mechanism. Initiation involves attack of a positive center on the exocyclic oxygen (the more basic oxygen) to form a dioxocarbocation (XLVIII). For example, for initiation by methyl carbocation derived from CH3 OSO2 CF3 or (CH3 2 I SbF 6

7-78

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THE MULTI-LAYER PERCEPTRON (MLP)

(n+1)

7-79

Cationic polymerization is not nearly as useful as anionic polymerization for synthesizing high-molecular-weight polyesters. The cationic route appears to be limited by intramolecular transesteri cation (cyclization) as well as other chain transfer to polymer reactions (including hydride and proton transfers) although there are few details in the literature. However, molecular weights in the 100,000 range have been observed for the highly reactive monomer b-propiolactone. The highly strained b-propiolactone undergoes a mixture of alkyl oxygen and acyl oxygen cleavages under some reaction conditions. Cationic ROP of lactones in the presence of an alcohol proceeds by an activated monomer mechanism similar to that for cyclic ethers (Sec. 7-2b-3-b) [Endo et al., 2002; Lou et al., 2002]. Propagation proceeds by nucleophilic attack of the hydroxyl end group of a propagating chain on protonated (activated) monomer:

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