AbstractCO2 capture from major stationary emission sites has been studied widely with the increasing realization of the negative impact of greenhouse gas emissions on climate change. In terms of capture technology, solvent scrubbing, membrane processes and adsorption processes are the major contenders with the latter making significant progress over the last decade due to both improved adsorbent and process design and operation. As is well known, capturing CO2 from flue gases at coal-fired power stations by pressure/vacuum swing adsorption is complicated by the existence of significant amounts of water, SOx, NOx and other impurities, which are detrimental to most commercial CO2 selective-adsorbents. Conventional adsorption-based CO2 capture processes rely on using a pre-treatment stage to remove water, SOx and NOx, which adds considerably to the overall cost. In contrast, we report here an adsorption process developed in our laboratory which directly tackles the untreated flue gas without a separate pre-treatment stage by using a propriety multiple-layered bed comprising different adsorbents. The species CO2, H2O, SOx and NOx are processed in the same column within different function layers optimized according to adsorption properties and process conditions. A fully programmable logic controller (PLC) automated three-column pilot plant was built to perform the study with real-time control and data acquisition conducted through Human Machine Interface/Supervisory Control and Data Acquisition (HMI/SCADA) system. Through running continuous experiments, the effects of impurities on process performance such as CO2 purity, recovery and process power are investigated and reported. This is the first in-depth report of the performance of adsorption based capture plants in the presence of impurities found in real flue gas streams.