Experimental evaluation of effect of oxidative degradation of aqueous monoethanolamine on heat of CO2 absorption, vapor liquid equilibrium and CO2 absorption rate

摘要

Oxidative degradation produces carboxylic acids which are one of the undesirable degradation products and may have a negative impact on the CO2 separation energy of post combustion capture system. 30wt% MEA solutions mixed with carboxylic acids were regarded as a simulated solution for degraded MEA and effect of the additives on heat of CO2 absorption, equilibrium CO2 loading and CO2 absorption rate were experimentally evaluated by using a differential reaction calorimetry (DRC) apparatus, a pressurized vessel to obtain vapor liquid equilibrium (VLE) data and a gas-liquid contactor, respectively. At the range of CO2 loading from 0.0 to 0.3 mol-CO2/mol-amine, the heat of CO2 absorption of the simulated solution increased by around 10% compared to the normal MEA solution. Moreover, the changing-point of the heat of CO2 absorption of the simulated solution moved to a leaner CO2 loading compared to the normal solution. Result of a ~(13)C-NMR analysis also indicated the change in reaction mechanism. At the absorber condition, the equilibrium CO2 loading of the simulated solution decreased by 20% in comparison with the normal solution, where it decreased by 10% at the stripper condition and therefore the cyclic CO2 loading also decreased. Both CO2 absorption rates decreased linearly but in different gradients with increasing CO2 loading. Higher pH in the simulated solution kept higher CO2 absorption rate, which is consistent with the result of pH measurement.