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The pressure effect on the carbonation behavior of CaO as model compound is studied under mild hydrothermal conditions, as relevant to sustainable geological CO2 sequestration and for potential utilization in thermochemical energy storage. Reaction yields are determined experimentally by means of in situ powder X‐ray diffraction using CaO powder samples in a controlled reaction with CO2 under gas pressures between 1.0 and 5.0 MPa and at temperatures between 298 and 373 K. The results show a two‐step conversion of CaO to CaCO3, involving Ca(OH)2 as a reactive intermediate, with differing influences of the microstructures on the individual reaction sub‐steps. A kinetic evaluation of the experimental data delivers a high rate‐enhancing effect of temperature on the hydration reaction, whereas the CaCO3 formation is strongly dependent on the available CO2 gas pressure. With this systematic investigation the optimal pressure and temperature conditions for this reaction system can be determined delivering a contribution to a sustainable climate and energy management.

Thermochemical energy storage is considered as an auspicious method for the recycling of medium-temperature waste heat. The reaction couple Mg(OH)2–MgO is intensely investigated for this purpose, suffering so far from limited cycle stability. To overcome this issue, Mg(OH)2, MgCO3, and MgC2O4·2H2O were compared as precursor materials for MgO production. Depending on the precursor, the particle morphology of the resulting MgO changes, resulting in different hydration behavior and cycle stability. Agglomeration of the material during cyclization was identified as main reason for the decreased reactivity. Immersion of the spent material in liquid H2O decomposes the agglomerates restoring the initial reactivity of the material, thus serving as a regeneration step.

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