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Sections 5.6.2 and 5.6.3 dealt with the deposition of metals from complexes; these processes follow the simple laws dealt with in Sections 5.2 and 5.3, particularly if they take place at mercury electrodes. The deposition of metals at solid electrodes (electrocrystallization) and their oxidation is connected with the kinetics of transformation of the solid phase, which has a specific character. A total of five different cases can be distinguished in these processes: 1. The deposition occurs at an electrode of a different metal or other conductive material (e.g. graphite). 2. The deposition occurs at an electrode of the same metal. 3. The metal is ionized in the anodic process to produce soluble ions. 4. The metal is anodically oxidized to ions that react with the components of the solution to yield an insoluble compound forming a surface film on the electrode. 5. A component of the solution participates in the anodic oxidation of the metal, so that the metal is converted directly into a surface film. These processes either lead to the formation of a new solid phase or the original solid phase grows or disappears. In addition to the electrochemical laws discussed earlier, this group of phenomena must be explained on the basis of the theory of new phase formation (crystallization, condensation, etc.). The basic properties of electrocrystallization can best be illustrated by the example of the deposition of a metal on an electrode of a different material (case 1).

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Dynamics of photochemical phase transition of guest/host liquid crystals with an azobenzene derivative as a photosensitive chromophore Chem Mater 14:385 391 Suzuki A, Tanaka T 1990 Phase transition in polymer gels induced by visible light Nature 346:345 347 Suzuki A, Ishii T, Maruyama Y 1996 Optical switching in polymer gels J Appl Phys 80:131 136 Tabiryan N, Serak S, Dai XM, Bunning T 2005 Polymer lm with optically controlled form and actuation Opt Express 13:7442 7448 Tammer M, Li J, Komp A, Finkelmann H, Kremer F 2005 FTIR spectroscopy on segmental reorientation of a nematic elastomer under external mechanical elds Macromol Chem Phys 206:709 714 Tanchak OM, Barrett CJ 2005 Light induced reversible volume changes in thin lms of azo polymers: the photomechanical effect Macromolecules 38:10566 10570 Tazuke S, Kurihara S, Ikeda T 1987 Ampli ed image recording in liquid crystal media by means of photochemically triggered phase transition.

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The formation of a new phase requires that the system be metastable, such as a supersaturated vapour prior to condensation, a supersaturated solution prior to crystallization, etc. The metastable situation of the system required for the formation of a new phase through an electrode reaction is brought about by the overpotential. At a suitable value of the excess energy in the system nuclei of the new phase are formed. If these nuclei are too small, then they become unstable as a result of the relatively high surface energy and decompose spontaneously. If their dimensions exceed a certain critical value, which is a function of the excess energy of the system, then they begin to grow spontaneously. Their formation requires a sufficiently large fluctuation of the variables of state of the system or the presence of sites at the interface at which nuclei can be formed with an overall decrease in the surface energy. The nucleation belongs to those processes where the individual events (of stochastic nature) occurring on the molecular level can be observed because of amplifying by subsequent macroscopic processes. Assume that current is passed either through the total nucleus surface area or through part thereof, such as the edge of a two-dimensional nucleus of monoatomic thickness. The transition of the ion M z+ to the metallic state obeys the equation for an irreversible electrode reaction, i.e. Eqs (5.2.12), (5.2.23) and (5.2.37). The effect of transport processes is neglected. The current density at time t thus depends on the number of nuclei and their active surface area. If there is a large number of nuclei, then the dependence of their number on time can be considered to be a continuous function. For the overall current density at time t we have -r)vndr (5.8.1)

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Chem Lett 16:911 914 Terentjev EM 1999 Liquid crystalline elastomers J Phys Condens Matter 11:R239 R257..

where A = zFkexp( azFrj/RT)cMz+ and A is the active surface area of a single nucleus. The rate of nucleation vn = dNjdt then gives the increase in the number of nuclei per unit time. The simplest case occurs when a number of nuclei N is formed at the beginning of the process and does not change with time (instantaneous nucleation). This is the case when the electrolysis is carried out by the double-pulse potentiostatic method (Fig. 5.18B), where the crystallization nuclei are formed in the first high, short pulse and the electrode reaction then occurs only at these nuclei during the second, lower pulse. A second situation in which instantaneous nucleation can occur is when the nuclei occupy all the active sites on the electrode at the beginning of the electrolysis. For instantaneous nucleation Eq. (5.8.1) assumes the form (5.8.2) Hemispherical nuclei will be considered; this case is important for the

Thomsen DL, Keller P, Naciri J, Pink R, Jeon H, Shenoy D, Ratna BR 2001 Liquid crystal elastomers with mechanical properties of a muscle Macromolecules 34: 5868 5875 Tsutsumi O, Shiono T, Ikeda T, Galli G 1997 Photochemical phase transition behavior of nematic liquid crystals with azobenzene moieties as both mesogens and photosensitive chromophores J Phys Chem B 101:1332 1337 Tsutsumi O, Demachi Y, Kanazawa A, Shiono T, Ikeda T, Nagase Y 1998a Photochemical phase transition behavior of polymer liquid crystals induced by photochemical reaction of azobenzenes with strong donor acceptor pairs J Phys Chem B 102:2869 2874 Tsutsumi O, Kitsunai T, Kanazawa A, Shiono T, Ikeda T 1998b Photochemical phase transition behavior of polymer azobenzene liquid crystals with electron donating and accepting substituents at 4,4u positions Macromolecules 31:355 359 Van der Veen G, Prins W 1971 Photomechanical energy conversion in a polymer membrane Nature Phys Sci 230:70 72.

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