The idea of this work is to reduce the negative effect of ordinary Portland cement (OPC) manufacture on the environment by decreasing clinker production temperature and developing an alternative rankinite binder that hardens in the CO2 atmosphere. The common OPC raw materials, limestone and mica clay, if they contain a higher MgO content, have been found to be unsuitable for the synthesis of CO2-curing low-lime binders. X-ray diffraction analysis (ex-situ and in-situ in the temperature range of 25–1150 °C) showed that akermanite Ca2Mg(Si2O7) begins to form at a temperature of 900 °C. According to Rietveld refinement, the interlayer distances of the resulting curve are more accurately described by the compound, which contains intercalated Fe2+ and Al3+ ions and has the chemical formula Ca2(MgO0.495·FeO0.202·AlO0.303)·(FeO0.248·AlO·Si1.536·O7). Stoichiometric calculations showed that FeO and Al2O3 have replaced about half of the MgO content in the akermanite structure. All this means that only ~4 wt% MgO content in the raw materials determines that ~60 wt% calcium magnesium silicates are formed in the synthesis product. Moreover, it was found that the formed akermanite practically does not react with CO2. Within 24 h of interaction with 99.9 wt% of CO2 gas (15 bar), the intensity of the akermanite peaks does not practically change at 25 °C; no changes are observed at 45 °C, either, which means that the chemical reaction does not take place. As a result, the compressive strength of the samples compressed from the synthesized product and CEN Standard sand EN 196-1 (1:3), and hardened at 15 bar CO2, 45 °C for 24 h, was only 14.45 MPa, while the analogous samples made from OPC clinker obtained from the same raw materials yielded 67.5 MPa.