Results for mass transfer in a rotating spiral device are presented here for absorption of carbon dioxide from nitrogen carrier gas using mixtures of diethanolamine (DEA) and water. The ability of the device to examine the full range of flow rate ratio for the two phases while controlling the relative thicknesses of the phase layers is applied to surveying absorption performance over a wide range of DEA concentration at 312 K and 1.8 bara. Comparisons are made for a fixed 86 mu m liquid layer thickness, which is shown to fix also the fraction of the liquid accessible by diffusion, while maintaining 90% removal of CO2 from a gas stream of 10% (mole) CO2 in nitrogen. The increasing liquid viscosity with DEA fraction is countered by reducing the liquid flow rate to maintain constant liquid layer thickness and diffusion depth. The allowed gas throughput, while meeting 90% removal, increases with DEA concentration until the increasing viscosity gives sufficient reduction in liquid flow rate to offset the increasing CO2 capacity of the liquid. The maximum gas flow rate has a broad peak centred at a DEA mole fraction of about 0.072 (31% by mass). Utilisation of the amine is increased as DEA concentration increases, apparently as a result of the longer residence time, suggesting an effect of chemical time scales on the order of seconds. For a fixed concentration, full utilisation of the amine is achieved by decreasing the liquid flow rate, which reduces layer thickness and increases diffusion time. The work highlights the use of the rotating spiral for rapid and accurate testing to determine optimum liquid composition of absorbent formulations. (C) 2016 Elsevier B.V. All rights reserved.