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(a) (b) Fig. 5.58 Scheme of a photogalvanic cell. The homogeneous photoredox process takes place in the vicinity of the optically transparent anode (a) or cathode (b) The two-electron oxidation of the dye is not very common; other dyes usually undergo one-electron redox reactions. The cathodic reaction (taking place in the non-illuminated cell compartment) regenerates the complementary redox system: Fe 3+ + e"- Fe 2 + (5.10.12) According to the reactions (5.10.9)-(5.10.12), we can classify this cell as a regenerative (AG = 0) photogalvanic cell based on reductive quenching (Fig. 5.58a). Good performance of the iron-thionine cell is conditioned by the generation of *Thi+ (and Leu2+) in close vicinity (below ca. 1 jum) of the anode; this can be achieved by using an optically transparent (e.g. SnO2) anode as a window (Fig. 5.58). The selectivity of the anode and cathode for the desired reactions (5.9.24) and (5.9.25) may be further increased by selecting the proper electrode materials or by chemical modification of the anode. A regenerative photogalvanic cell with oxidative quenching (Fig. 5.58b) is based, for example, on the Fe 3+ -Ru(bpy)| + system. In contrast to the iron-thionine cell, the homogeneous photoredox process takes place near the (optically transparent) cathode. The photoexcited *Ru(bpy)l+ ion reduces Fe3+ and the formed Ru(bpy)3+ and Fe 2+ are converted at the opposite electrodes to the initial state. More complicated photogalvanic cells may employ two light absorbing systems: one in the cathodic process and the other in the anodic process. An
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397 interesting example is a cell with two different chlorophyll-based absorbers. The cathodic process starts by photoexcitation of a modified natural chloroplast with deactivated photosystem II (PS II for terminology of photosynthetic processes see page 469). The remaining PS I reduces, for example, anthraquinone-2-sulphonate. The regenerative cycle of PS I is linked to tetramethyl-p-phenylenediamine which is cycled at the cathode. The complementary anodic process is O2 evolution by the action of a second chloroplast system with active PS II; electrons from photoexcited PS II are transferred to the tetramethyl-p-phenylenediamine and the cycle is terminated by its oxidation at the anode. The whole cell resembles photosynthesis, the net output being O2 and reduced anthraquinone-2-sulphonate (cf. Section 6.5.2). The efficiency of the photocurrent generation in practical photogalvanic cells is generally low, since it is limited by short lifetimes of the excited dyes, parasitic electron transfer reactions, etc. The importance of the photogalvanic effect rests in basic electrochemical research of homogeneous photoredox reactions. To this purpose, original experimental techniques have been developed, e.g. voltammetry with an optically transparent rotating disk electrode. The photoexcitation of reactants makes the study of redox reactions possible in a considerably broader region of the Gibbs free energy changes than with the ground-state reactants. This brings interesting conclusions, for example, for the formulation of a more general theory of electron transfer, preparation of compounds in less-common oxidation states, etc. 5.10.4 Semiconductor photoelectrochemistry and photovoltaic effects Basic properties of semiconductors and phenomena occurring at the semiconductor/electrolyte interface in the dark have already been discussed in Sections 2.4.1 and 4.5.1. The crucial effect after immersing the semiconductor electrode into an electrolyte solution is the equilibration of electrochemical potentials of electrons in both phases. In order to quantify the dark- and photoeffects at the semiconductor/electrolyte interface, a common reference level of electron energies in both phases has to be defined. Let us choose, as an arbitrary reference level, the energy of an electron at rest in vacuum, e0 (cf. Section 3.1.2). This reference energy is obvious in studies of the solid phase, but for the liquid phase, the Trasatti's conception of 'absolute electrode potentials' (Section 3.1.5) has to be adopted. The formal energy levels of the electrolyte redox systems, REDOX, referred to (), are given by the relationship:
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