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Fig. 5.61 Current density-potential characteristics of n-semiconductor electrode in the dark and upon illumination
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Fig. 5.62 Scheme of a photovoltaic cell with nsemiconductor photoanode the p-semiconductor electrode as a photocathode. The most common photovoltaic cells are based on the combination of a semiconductor photoanode and a metal cathode (Fig. 5.62). Cells with a metal anode and a semiconductor photocathode or with a semiconductor photoanode and a semiconductor photocathode have, however, also been described. The potential which controls the photoelectrochemical reaction is generally not the photopotential defined by Eqs (5.10.20) and (5.10.21) (except for the very special case where the values of * v, REDOX and the initial Fermi energy of the counterelectrode are equal). The energy which drives the photoelectrochemical reaction, R can be expressed, for example, for an n-semiconductor electrode as
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This energy is consumed to overcome the overpotentials of the electrode reactions (rja, rjc), the IR drop in the external circuit and electrolyte, and it might partly be converted into the free energy, AG, of stable products (if any) of the endoergic electrochemical reaction: R = e(r a + c + IR) + AG/NA (5.10.24) The electrochemical cell can again be of the regenerative or electrosynthetic type, as with the photogalvanic cells described above. In the regenerative photovoltaic cell, the electron donor (D) and acceptor (A) (see Fig. 5.62) are two redox forms of one reversible redox couple, e.g. Fe(CN)2~/4~, I 2 /I", Br 2 /Br", S2~/Sx~, etc. the cell reaction is cyclic (AG = 0, cf. Eq. (5.10.24) since D+=A and D=A~). On the other hand, in the electrosynthetic cell, the half-cell reactions are irreversible and the products (D+ and A~) accumulate in the electrolyte. The most carefully studied reaction of this type is photoelectrolysis of water (D+ = O2 and y4~ = H2). Other photoelectrosynthetic studies include the preparation of S2OI , the reduction of CO2 to formic acid, N2 to NH3, etc. The photoelectroiysis of water was first studied in 1971 by A. Fujisima
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and K. Honda, who used a n-TiO2 photoanode and a Pt counterelectrode. From the band positions and the formal energy levels of the H + /H 2 and O2/H2O couples (Fig. 5.59), it is, nevertheless, apparent that the cell: n-TiO2 |aqueous electrolyte| Pt (5.10.25) does not provide sufficient voltage for photoelectrolysis of water (1.229 V) since the energy level of hydrogen electrode at pH 7 is about 0.2 V above the conduction band edge (this difference remains constant also at other pH values since both energy levels show the same Nernstian shift with pH). The missing voltage has, therefore, to be supplied either from an external source (photoassisted electrolysis of water) or by immersing the electrodes into electrolytes of different pH values (photoanode in alkaline and cathode in acidic electrolyte, the electrolytes being separated by a suitable membrane). The direct photoelectrolysis of water requires that the ey level be below the O2/H2O level and the ec level be above the H + /H 2 level. This condition is satisfied, e.g. for CdS, GaP, and several large-band gap semiconductors, such as SrTiO3, KTaO3, Nb2O5 and ZrO2 (cf. also Fig. 5.59). From the practical points of view, these materials show, however, other specific problems, e.g. low electrocatalytic activity, sensitivity to photocorrosion (CdS, GaP), and inconvenient absorption spectrum (oxides). The world-wide effort in photo(electro)chemical splitting of water started in the 1970s. It was motivated by two factors: (1) the oil crisis which stimulated the research in the solar energy conversion, and (2) the optimism connected with the 'hydrogen economy'. At present, however, the conversion of solar energy via photo(electro)lysis of water as well as the use of hydrogen as a medium for the energy storage and transport do not seem to compete seriously with the currently available energy resources. 5.10.5 Sensitization of semiconductor electrodes The band-gap excitation of semiconductor electrodes brings two practical problems for photoelectrochemical solar energy conversion: (1) Most of the useful semiconductors have relatively wide band gaps, hence they can be excited only by ultraviolet radiation, whose proportion in the solar spectrum is rather low. (2) the photogenerated minority charge carriers in these semiconductors possess a high oxidative or reductive power to cause a rapid photocorrosion. Both these disadvantages can be overcome by sensitization. In this case, the light is not absorbed in the semiconductor phase, but in an organic or organometallic photoredox active molecule (sensitizer, S), whose excitation energy is lower than eg. The sensitizer might either be dissolved in the electrolyte or adsorbed at the semiconductor surface. If the redox levels of the sensitizer in the ground and excited states are properly positioned relative to the ec and v levels, a charge injection from the photoexcited sensitizer (S*) might occur. The photoexcited molecule reacts at the
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