Millimeter-sized spheres were prepared in this work as potential solid sorbents for industrial-scale CO2 capture due to their low cost, excellent adsorption capacity and reusability characters. The naturally abundant palygorskite was smashed with jet pulverization, and then acid treated to increase its surface area from 148 to 390 m(2)/g. Then the tetraethylenepentamine (TEPA) functionalized acid-modified palygorskite (MPA) was synthesized via chemical impregnation. In addition, MPA spheres (MPAS) with average size of similar to 3.6 mm were produced by a pellet machine. The prepared solid sorbents were characterized using X-ray diffraction (XRD), Fourier transformation infrared spectroscopy (FTIR), scanning electron microscopy (SEM), thermogravimetric analysis (TGA), and N-2 adsorption-desorption isotherms treated by BET (Brunauer-Emmett-Teller) analysis. The thermogravimetric analysis indicated that the CO2 adsorption capacity of nature palygorskite (0.63 mmol/g) could be enhanced through amine modification. The MPAS-50 had the best CO2 adsorption capacity (2.63 mmol/g) and excellent repeatable adsorption ability, according to the CO2 adsorption tests. The results indicated that the TEPA-functionalized palygorskite sphere is a promising solid sorbent for CO2 capture in industrial green house gases controlling fields.