The effects of carbonation of mechanochemically prepared C-S-H samples under ambient conditions for upto 6 months have been investigated by Raman spectroscopy and X-ray diffraction. The type and extent of carbonation are strongly dependent on the initial CaO/SiO2 (C/S) ratio of the samples. Amorphous calcium carbonate hydrate is formed within minutes upon exposure to air. It crystallizes, over time, to give primarily vaterite at C/S >= 0.67 and aragonite at C/S <= 0.50. Calcite was not observed as a primary carbonation product within the time frame investigated. Decalcification upon storage also initiates silicate polymerization. The dimeric silicate units seen in the calcium-rich phases polymerize rapidly to yield Q(2) silicate moieties. After 6 months, broad bands are seen in most spectra, ascribed to poorly ordered silica. C-S-H phases with C/S ratios of 0.75 and 0.67 are the most resistant to carbonation, and even after 6 months of storage, Q(2) silicate units still dominate their structures. The ability of Raman spectroscopy to probe the short-range order of poorly crystalline materials is ideal for investigations of C-S-H structure. Additionally, the technique's sensitivity toward the various calcium carbonate polymorphs illuminates the sequence of carbonation and decalcification processes during aging of C-S-H. Of particular importance is the identification of amorphous calcium carbonate as the first carbonation product. Additionally, the formation of aragonite as a carbonation product is related to the presence of SiO2 gel in the aged samples
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