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65 with it. This definition has changed somewhat over the years and the definitions have now been unified (Pure Applied Chemistry, 57, 531, 1985). As these definitions are based on pH measurement with the hydrogen electrode they will be discussed in Section 3.3.2. For the same reason the pH scales in non-aqueous solutions will be dealt with in Section 3.2.6. For solutions of extreme acidity (e.g. the H 2 O-H 2 SO 4 mixture) the acidity function Ho was introduced by L. P. Hammett as Ho = pATA(BH+) + log - ^ - = -log aH+ - log - ^ C

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30 45 Irradiation time (min)

(1.4.40)

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Figure 9.14. Changes in the depth of the dent as a function of photoirradiation time for CN-azopolymers (solid gures) and H-azopolymers (open gures). The numbers show the weight content of the azo moieties. The open crosses show the control experiment using PMMA. Source: Narita, 2007. Reprinted with permission.

V-NH-

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H-azopolymers, even though they contained different types of azobenzene. These results show that H-azopolymers could exhibit immobilization capabilities similar to CN-azopolymers, despite the differences in their chemical structures. Photoimmobilization of IgGs was achieved by performing photoirradiation for 30 min to examine the ef ciency of the immobilization process. The relative ef ciencies of the photoimmobilization processes on the different azopolymers were plotted as a function of their azobenzene contents, as shown in Fig. 9.15. The immobilization ef ciencies of both the CN- and H-azopolymers. increased with azobenzene content up to B30 wt% and then became saturated, although the saturated values were different between the CN- and H-azopolymers. This result indicates that an azobenzene moiety that exhibits photoisomerization is essential to immobilize IgGs on azopolymers when using a photoimmobilization process. Next, the authors con rmed the relationship between the immobilization of IgG and the deformation ef ciency of the azopolymer. The relative immobilization ef ciencies were plotted as a function of indent depth, as shown in Fig. 9.16. Incremental changes in the immobilization ef ciency were observed by increasing the depth of the indents. However, the immobilization ef ciency of the Hazopolymers was higher than that of the CN-azopolymers across the whole range, and this is also shown in Fig. 9.15. This difference shows that the degree of photoimmobilization is not only affected by the deformation capability but is also a property of the surface of the azopolymer and is related to the chemical structure of the azobenzene that is incorporated in the azopolymer. Whitesides and coworkers have also reported that immobilization is in uenced by the properties of the surface (Ostuni et al., 2001).

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The monomer and lower oligomers are soluble in the electrolyte, but with increasing polymerization degree the solubility decreases. After attaining some critical value, an insoluble film is formed on the anode. Lower (soluble) oligomers can also diffuse from the electrode into the bulk of the electrolyte, hence the faradaic yield of electrochemical polymerization is, at least in the primary stages, substantially lower than 100 per cent. The ideal electropolymerization scheme (Eq. (5.5.39)) is further complicated by the fact that lower oligomers can react with nucleophilic substances (impurities, electrolyte anions, and solvent) and are thus deactivated for subsequent polymerization. The rate of these undesired side reactions apparently increases with increasing oxidation potential of the monomer, for example, in the series: aniline < pyrrole < thiophene < furan < benzene The nucleophilic reaction with the solvent is of crucial importance. Monomers with lower oxidation potentials (aniline and pyrrole) can easily be polymerized even in aqueous electrolytes. For monomers with higher oxidation potentials, aprotic solvents must be used, such as acetonitrile

Relative efficiency of immobilization (%)

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