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Fig. 5.28
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Structure of glass-like carbon. (According to G. M. Jenkins and K. Kawamura)
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Carbon electrodes are widely used in electrochemistry both in the laboratory and on the industrial scale. The latter includes production of aluminium, fluorine, and chlorine, organic electrosynthesis, electrochemical power sources, etc. Besides the use of graphite (carbons) as a virtually inert electode material, the electrochemical intercalation deserves special attention. This topic will be treated in the next paragraph. In spite of the high effort focused on the carbon electrochemistry, very little is known about the electrochemical preparation of carbon itself. This challenging idea appeared in the early 1970s in connection with the cathodic reduction of poly(tetrafluoroethylene) (PTFE) and some other perfluorinated polymers. The standard potential of the hypothetical reduction of PTFE to elemental carbon: (CF2)n + 2e" + 2H + -> Cn + 2HF (5.5.28) estimated from the Gibbs free energies of formation (cf. Sections 3.1.4 and 3.1.5) equals 1.00 V at 25 C. The reductive carbonization of PTFE is, therefore, thermodynamically highly favoured, and it indeed occurs at the carbon/PTFE interface in aprotic liquid or solid electrolytes. The produced elemental carbon is termed electrochemical carbon. It is reversibly dopable (reducible) under insertion of supporting electrolyte cations into the carbon skeleton.
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316 It should be emphasized that the electrochemical carbonization proceeds, in contrast to all other common carbonization reactions (pyrolysis), already at the room temperature. This fact elucidates various surprising physicochemical properties of electrochemical carbon, such as extreme chemical reactivity and adsorption capacity, time-dependent electronic conductivity and optical spectra, as well as its very peculiar structure which actually matches the structure of the starting fluorocarbon chain. The electrochemical carbon is, therefore, obtained primarily in the form of linear polymeric carbon chains (polycumulene, polyyne), generally termed carbyne. This can be schematically depicted by the reaction: F F F F F" F" F~ F"
_ l _ l ( _ l( _ l _ ^ ~~^f"~ f~~ f~~(f~" * =O=C-C~C_
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(5.5.29)
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F F F F F" F" F" F~ The product of the reaction (5.5.29) is, however, unstable against subsequent interchain crosslinking and insertion of supporting electrolyte cations. The electrochemical carbonization of fluoropolymers was recently reviewed by L. Kavan. Insertion (intercalation) compounds. Insertion compounds are defined as products of a reversible reaction of suitable crystalline host materials with guest molecules (ions). Guests are introduced into the host lattice, whose structure is virtually intact except for a possible increase of some lattice constants. This reaction is called topotactic. A special case of topotactic insertion is reaction with host crystals possessing stacked layered structure. In this case, we speak about 'intercalation' (from the Latin verb intercalare, used originally for inserting an extra month, mensis intercalarius, into the calendar). The intercalated guest molecules have a tendency to fill up completely the particular interlayer space in the host crystal, rather than to occupy randomly distributed interstitial sites between the layers. A peculiarity of intercalation is that the sequence of filled and empty interlayer spaces is very often regular, i.e. the structure of intercalation compounds consists of stacked guest layers interspaced between a defined number of the host layers. The number of host layers corresponds to the so-called stages of intercalation compounds. Stage 1 denotes successively stacked host and guest layers, stage 2 denotes a system with two host layers between one guest layer, etc. This is schematically depicted in Fig. 5.29. Graphite crystal is the best known host material for intercalation reactions. The host layers are clearly defined by planes of carbon hexagons, also called graphene layers. (The term 'graphene' has been derived by analogy with condensed aromatic hydrocarbons: naphthalene, anthracene, tetracene, perylene, etc.). In contrast to other host materials (e.g. inorganic sulphides), graphite also forms compounds with high stage numbers
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