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Carbonate is one of the most abundant anions in ground water. It also appears as saturated concentration in the process water at LKAB, a mining company in the northern part of Sweden. Sorption of carbonate on magnetite (the major source of iron ore in this company) may affect the surface chemistry of the iron oxide by forming a carbonate surface instead of an oxide surface. This would affect the interactions between magnetite particles and other species dissolved in the process water. Attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR) has proved to be a useful technique in the study of adsorption/desorption properties of ions in mineral processing and environmental science. Magnetite was synthesized by coprecipitation of Fe II and Fe III in alkaline solution and deposited on a ZnS internal reflection element. Adsorption of carbonate on magnetite, and the effect of pH, Na, Ca, and silicate ions on the amount and speciation of adsorbed carbonate was monitored in situ. Adsorption of carbonate onto magnetite was found to increase with the acidity of the solution from pH 8.5 to pH 6.5 and also increased with increasing calcium concentration from 0 to 1.0 mM. The spectroscopy results were discussed and compared with previous findings in the literature.