Solid sorbents are essential for developing technologies that directly capture CO₂ from air. In solid sorbents, metal oxides and/or alkali metal carbonates such as potassium carbonate (K₂CO₃) are promising active components owing to their high thermal stability, low cost, and ability to chemisorb the CO₂ present at low concentrations in air. However, this chemisorption process is likely limited by internal diffusion of CO₂ into the bulk of K₂CO₃. Therefore, the size of the K₂CO₃ particles is expected to be an important factor in determining the kinetics of the sorption process during CO₂ capture. To date, the effects of particle size on supported K₂CO₃ sorbents are unknown mainly because particle sizes cannot be unambiguously determined. Here, we show that by using a series of techniques, the size of supported K₂CO₃ particles can be established. We prepared size-tuned carbon-supported K₂CO₃ particles by tuning the K₂CO₃ loading. We further used melting point depression of K₂CO₃ particles to collectively estimate the average K₂CO₃ particle sizes. Using these obtained average particle sizes, we show that the particle size critically affects the efficiency of the sorbent in CO₂ capture from air and directly affects the kinetics of CO₂ sorption as well as the energy input needed for the desorption step. By evaluating the mechanisms involved in the diffusion of CO₂ and H₂O into K₂CO₃ particles, we relate the microscopic characteristics of sorbents to their macroscopic performance, which is of interest for industrial-scale CO₂ capture from air.

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