This study presents a pilot-scale spray drying system designed to manufacture spherical mesoporous silica particles (MSP) that is capable of producing up to 100 g per hour. The MSP fabricated via a nozzle pressure of 4 kg/cm(2) and a drying temperature of 200 degrees C possess a high specific area of 1012 m(2)/g, a narrow pore size distribution with an average pore diameter of 2.4 nm, and large pore volume of 0.81 cm(3)/g. They were further modified with a tetraethylenepentamine (TEPA-MSP) to enhance CO2 adsorption selectivity from gas streams. The adsorption capacity of 15% CO2 on TEPA-MSP was significantly influenced by adsorption temperature and water vapor of air streams, and reached a maximum of 87.05 mg/g (1.98 mmol/g) at 60 degrees C and 129.19 mg/g (2.94 mmol/g) at a water vapor of 6.98%. The adsorption capacities and the physicochemical properties of TEPA-MSP were preserved through 20 cycles of adsorption-desorption operation. A comparative study revealed that the TEPA-MSP had better adsorption performance of 15% CO2 than the TEPA-modified granular activated carbon and zeolite. These results suggest that the TEPA-MSP can be stably employed in the prolonged cyclic CO2 adsorption and that they possess good potential for CO2 capture from flue gas. (C) 2012 Elsevier B. V. All rights reserved.