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Baizer, M. and H. Lund (Eds), Organic Electrochemistry, M. Dekker, New York, 1983. Fleischmann, M., and D. Pletcher, Organic electrosynthesis, Roy. Inst. Chem. Rev., 2, 87 (1969). Fry, A. J., Synthetic Organic Electrochemistry, John Wiley & Sons, Chichester, 1989. Fry, A. J., and W. E. Britton (Eds), Topics in Organic Electrochemistry, Plenum Press, New York, 1986. Kyriacou, D. K., and D. A. Jannakoudakis, Electrocatalysis for Organic Synthesis, Wiley-Interscience, New York, 1986. Lamy, C , see page 368. Peover, M. E., Electrochemistry of aromatic hydrocarbons and related substances, in Electroanalytical Chemistry (Ed. A. J. Bard), Vol. 2, p. 1, M. Dekker, New York, 1967. Shono, T., Electroorganic Chemistry as a New Tool in Organic Synthesis, SpringerVerlag, Berlin, 1984. Torii, S., Electroorganic Syntheses, Methods and Applications, Kodansha, Tokyo, 1985. Weinberg, N. L. (Ed.), Techniques of Electroorganic Synthesis, Wiley-Interscience, New York, Part 1, 1974, Part 2, 1975. Weinberg, N. L., and H. R. Weinberg, Oxidation of organic substances, Chem. Rev., 68,449(1968). Yoshida, K., Electrooxidation in Organic Chemistry, The Role of Cation Radicals as Synthetic Intermediates, John Wiley & Sons, New York, 1984. Zuman, P., Substitution Effects in Organic Polarography, Plenum Press, New York, 1967.
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Photoelectrochemistry Classification of photoelectrochemical phenomena
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Photoelectrochemistry studies the effects occurring in electrochemical systems under the influence of light in the visible through ultraviolet region. Light quanta supply an extra energy to the system, hence the electrochemical reactions, which are thermodynamically or kinetically suppressed in the dark, may proceed at a high rate under illumination. (There also exists an opposite effect, where the (dark) electrochemical reactions lead to highly energetic products which are able to emit electromagnetic radiation. This is the principle of 'electrochemically generated luminescence', mentioned in Section 5.5.6.) Two groups of photoelectrochemical effects are traditionally distinguished: photogalvanic and photovoltaic. The photogalvanic effect is based on light absorption by a suitable photoactive redox species (dye) in the electrolyte solution. The photoexcited dye subsequently reacts with an electron donor or acceptor process, taking place in the vicinity of an electrode, is linked to the electrode
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391 reaction which restores the original form of the dye. The cycle is terminated by a counterelectrode reaction in the non-illuminated compartment of the cell. Both electrode reactions may (but need not) regenerate the reactants consumed at the opposite electrodes. The photopotential and photocurrent appear essentially as a result of concentration gradients introduced by an asymmetric illumination of the photoactive electrolyte solution between two inert electrodes. Therefore, any photogalvanic cell can, in principle, be considered as a concentration cell. The photovoltaic effect is initiated by light absorption in the electrode material. This is practically important only with semiconductor electrodes, where the photogenerated, excited electrons or holes may, under certain conditions, react with electrolyte redox systems. The photoredox reaction at the illuminated semiconductor thus drives the complementary (dark) reaction at the counterelectrode, which again may (but need not) regenerate the reactant consumed at the photoelectrode. The regenerative mode of operation is, according to the IUPAC recommendation, denoted as 'photovoltaic cell' and the second one as 'photoelectrolytic cell'. Alternative classification and terms will be discussed below. The term 'photovoltaic effect' is further used to denote nonelectrochemical photoprocesses in solid-state metal/semiconductor interfaces (Schottky barrier contacts) and semiconductor/semiconductor {pin) junctions. Analogously, the term 'photogalvanic effect' is used more generally to denote any photoexcitation of the d.c. current in a material (e.g. in solid ferroelectrics). Although confusion is not usual, electrochemical reactions initiated by light absorption in electrolyte solutions should be termed 'electrochemical photogalvanic effect', and reactions at photoexcited semiconductor electodes 'electrochemical photovoltaic effect'. The boundary between effects thus defined is, however, not sharp. If, for instance, light is absorbed by a layer of a photoactive adsorbate attached to the semiconductor electrode, it is apparently difficult to identify the light-absorbing medium as a 'solution' or 'electrode material'. Photoexcited solution molecules may sometimes also react at the photoexcited semiconductor electrode; this process is labelled photogalvanovoltaic effect. The electrochemical photovoltaic effect was discovered in 1839 by A. E. Becquerelt when a silver/silver halide electrode was irradiated in a solution of diluted HNO3. Becquerel also first described the photogalvanic effect in a cell consisting of two Pt electrodes, one immersed in aqueous and the other in ethanolic solution of Fe(ClO4)3. This discovery was made about the same time as the observation of the photovoltaic effect at the Ag/AgX electrodes. The term 'Becquerel effect' often appears in the old literature, even for denoting the vacuum photoelectric effect which was discovered almost 50 years later. The electrochemical photovoltaic effect was elucidated in 1955 by W. H. Brattain and G. G. B. Garrett; the theory was further developed
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