Multishelled CaO Microspheres Stabilized by Atomic Layer Deposition of Al2O3 for Enhanced CO2 Capture Performance

CO₂ capture and storage is a promising concept to reduce anthropogenic CO₂ emissions. The most established technology for capturing CO₂ relies on amine scrubbing that is, however, associated with high costs. Technoeconomic studies show that using CaO as a high-temperature CO₂ sorbent can significantly reduce the costs of CO₂ capture. A serious disadvantage of CaO derived from earth-abundant precursors, e.g., limestone, is the rapid, sintering-induced decay of its cyclic CO₂ uptake. Here, a template-assisted hydrothermal approach to develop CaO-based sorbents exhibiting a very high and cyclically stable CO₂ uptake is exploited. The morphological characteristics of these sorbents, i.e., a porous shell comprised of CaO nanoparticles coated by a thin layer of Al₂O₃ (<3 nm) containing a central void, ensure (i) minimal diffusion limitations, (ii) space to accompany the substantial volumetric changes during CO₂ capture and release, and (iii) a minimal quantity of Al₂O₃ for structural stabilization, thus maximizing the fraction of CO₂-capture-active CaO.

CaO-based CO₂ sorbents featuring a high CO₂ uptake (0.55 g_CO2 g_sorbent⁻¹) are developed via a template-assisted synthesis approach. The highly porous, nanostructured multishelled morphology is stabilized by an ultrathin film of Al₂O₃ grown by atomic layer deposition. The capacity retention is 89.9% after 30 operation cycles.

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