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

Abstract 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.