In this work, a computational study was performed on the adsorption separation of CO2 from flue gases (mixtures Of CO2/N-2/O-2) in Cu-BTC metal-organic framework (MOF) to investigate the applicability of MOFs to this important industrial system. The computational results showed that Cu-BTC is a promising material for separation Of CO2 from flue gases, and the macroscopic separation behaviors of the MOF were elucidated at a molecular level to give insight into the underlying mechanisms. The present work not only provided useful information for understanding the separation characteristics of MOFs, but also showed their potential applications in chemical industry. (C) 2007 American Institute of Chemical Engineers.