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Solid solutions of lithium and potassium metazirconates Li_2−xK_xZrO₃ (where, 0⩽x⩽2) were prepared by coprecipitation. Samples were characterized by powder X-ray diffraction, scanning electron microscopy, and thermogravimetric analyses. Results showed that the solubility limits of potassium into Li₂ZrO₃ is x=0.2. Furthermore, at higher potassium concentrations, a new phase was synthesized, Li_2.27K_1.19Zr_2.16O_6.05. For structural studies of this new phase, XRD data were analyzed by Rietveld refinements. Additionally, at high potassium concentrations different phases of ZrO₂ were found, as potassium tends to sublimate. On the other hand, lithium–potassium metazirconate solid solutions, Li_2−xK_xZrO₃, were tested as CO₂ captors. Thermal analyses into a CO₂ flux showed that Li_2−xK_xZr₂O₃ solid solutions present a better CO₂ absorption than Li₂ZrO₃ pure. The differences observed in the CO₂ sorption …