Direct capture of carbon dioxide from air via lime-based sorbents

Abstract

Direct air capture (DAC) is a developing technology for removing carbon dioxide (CO2) from the atmosphere or from low-CO2-containing sources. In principle, it could be used to remove sufficient CO2 from the atmosphere to compensate for hard-to-decarbonize sectors, such as aviation, or even for polishing gas streams containing relatively low CO2 concentrations. In this paper, the performance of lime-based sorbents for CO2 capture from air in a fixed bed was investigated. The effects of sorbent type, particle diameter, air flow rate, and relative humidity on the breakthrough time, breakthrough shape, and global reaction rate over a series of capture and regeneration cycles were examined. The greatest reaction rates and conversions were obtained when the sorbents were pre-hydrated and inlet air was humidified to 55% relative humidity. Humidifying the air alone leads to axial carbonation gradients since there is competition between CO2 and water with the available CaO. Negligible conversion, over the duration of the experiment, is obtained in a dry system without pre-hydration and humid air. A shrinking-core gas–solid reaction model was fitted to the breakthrough curves in order to estimate the surface reaction and effective diffusion constants. Although the surface reaction constants of the two sorbents were similar, the pelletized limestone had a greater effective diffusivity due to its greater porosity. At mild calcination conditions with air at 850 °C, the pelletized particles maintained their activity over nine carbonation–calcination cycles with a conversion drop of only 9% points.