Optimization of the structural characteristics of CaO and its effective stabilization yield high-capacity CO sorbents.

Calcium looping, a CO capture technique, may offer a mid-term if not near-term solution to mitigate climate change, triggered by the yet increasing anthropogenic CO emissions. A key requirement for the economic operation of calcium looping is the availability of highly effective CaO-based CO sorbents. Here we report a facile synthesis route that yields hollow, MgO-stabilized, CaO microspheres featuring highly porous multishelled morphologies. As a thermal stabilizer, MgO minimized the sintering-induced decay of the sorbents' CO capacity and ensured a stable CO uptake over multiple operation cycles. Detailed electron microscopy-based analyses confirm a compositional homogeneity which is identified, together with the characteristics of its porous structure, as an essential feature to yield a high-performance sorbent. After 30 cycles of repeated CO capture and sorbent regeneration, the best performing material requires as little as 11 wt.% MgO for structural stabilization and exceeds the CO uptake of the limestone-derived reference material by ~500%.