“…Calcium oxide (CaO) has been considered as the most advantageous CO 2 -sorbent within the mixed oxides family (Mg, Zn, Cu, K, Al, and Ca) because it carbonates (CBN, ) over a wider range of adsorption temperatures (200–700 °C), is easily available at a competitive price, , and is regenerated by calcination, even though it undergoes a strong reduction of sorption capacity under cyclic carbonation/calcination usage, because of sintering. − To face this issue, CaO is utilized in combined forms with inert stabilizers: dolomite is a natural material with this feature, while the literature refers to the synthetic CaO-based materials, with different inert phases (Al 2 O 3 or calcium–aluminates Ca x Al y O z above all). In situ CO 2 separation, that is, capture of CO 2 simultaneously to its production, was proposed as a promising strategy, , applicable to chemical looping combustion of hydrocarbons, , gasification with calcium looping cycle, − steam reforming of methane (SMR, ) ,− or higher hydrocarbons (SR, ). − Besides the net reduction of CO 2 emissions, the in situ CO 2 capture brings in an additional advantage, known as “sorption-enhancing”: the subtraction of CO 2 from the gaseous reaction environment displaces the equilibria of the water gas shift (WGS, ) and then of steam reforming (, ) toward products, therefore increasing outlet H 2 purity. All this considered, exploitation of CaO as CO 2 -sorbent appears as a versatile and promising practice to face the ever more urging issues related to climate change mitigation. − The effective application on a large scale needs experimental testing of efficient materials and technologies, as well as the refinement of modeling tools, in order to get reliable predictions of the CaO peculiar dynamic behavior in CBN () processes. This work is focused on the latter field.…”