The rational design of functionalized porous metal organic frameworks (MOFs) for gas adsorption applications has been applied using three spacer ligands H2DPT (3,6-di(pyridin-4-yl)-1,4-dihydro-1,2,4,5-tetrazine), DPT (3,6-di(pyridin-4-yl)-1,2,4,5-tetrazine), and BPDH (2,5-bis(4-pyridyl)-3,4-diaza-2,4-hexadiene) to synthesize TMU-34, [Zn(OBA)(H2DPT)(0.5)](n)center dot DMF, TMU-34(-2H), [Zn(OBA)(DPT)(0.5)]center dot DMF, and TMU-5, [Zn(OBA)(BPDH)(0.5)](n) center dot 1.5DMF, respectively. By controlling the pore size and chemical functionality of these three MOFs, we can improve the interactions between CO, and especially CH4 with the frameworks. Calculated Q(st)(CH4) for TMU-5, TMU-34, and TMU-34(-2H) are 27, 23, and 22 kJ mol(-1), respectively. These Q(st) values are among the highest for CH4- framework interactions. For systematic comparison, two reported frameworks, TMU-4 and TMU-5, have been compared with TMU-34 and TMU-34(-2H) in CO2 adsorption.