The structure modification of metal–organic frameworks (MOFs) is a promising technique to enhance its selective adsorption of carbon dioxide at room temperatures. However, to date, little is known on the structure-property relationship of MOFs for carbon capture. In this work, the effects of chemical composition of MOFs on selective adsorption of carbon dioxide were studied systematically. A series of aluminum-based MIL-53 with similar formula units but different organic ligands, Al(OH)BDC-X [BDC = terephthalate, X = H, NH2, NO2, 2(CH3)], were...