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Electrochemical measurements were associated with Fourier transform infrared spectroscopy, Raman microprobe, scanning electron microscopy and X-ray diffraction to study the behavior of carbonate green rust/Fe(III) redox system, in carbonate solutions. Carbonate green rust undergoes a reversible oxidation, leading to the transformation of Fe(II) present in its structure into Fe(III). This oxidation does not involve a dissolution/precipitation mechanism, but a solid-state transformation. Two oxidized products have been detected, normalFefalse(III)1 and normalFefalse(III)2. normalFefalse(III)1 is the first ferric product resulting from the oxidation of carbonate green rust; it undergoes a structural rearrangement that leads to its gradual conversion into a more stable product, normalFefalse(III)2. The kinetics of the normalFefalse(III)1 -to- normalFefalse(III)2 transformation were investigated. It allowed us to explain the evolution of the potential during the oxidation by air of a carbonate green rust suspension. © 2003 The Electrochemical Society. All rights reserved.

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