Timescales for the Spray-Mediated Gas Exchange of Carbon Dioxide

The air–sea exchange of carbon dioxide (CO2) on a global scale is a key factor in understanding climate change and predicting its effects. The magnitude of sea spray’s contribution to this flux is currently highly uncertain. Constraining CO2’s diffusion in sea spray droplets is important for reducing error margins in global estimates of oceanic CO2 uptake and release. The timescale for CO2 gas diffusion within sea spray is known to be shorter than the timescales for the droplets’ physical changes to take place while aloft. However, the rate of aqueous carbonate reactions relative to these timescales has not been assessed. This study investigates the timescales of droplet physical changes to those of chemical transformations across the H2CO3/HCO3−/CO32− sequence. We found that physical timescales are rate limiting and that evaporation drives carbonate species into gaseous CO2, promoting the production and evasion of CO2 from sea spray droplets. This has important implications for carbon cycling and feedback in the surface ocean.