We nevertheless computed the energetics of O2 chemisorption and found it to be favorable in these MOFs but at the cost of fairly high oxo formation barriers with O2 when CO is used as a coreductant (Supporting Information Text S2 and Figures ). This suggests the potential of the three identified Mn MOFs to use benign O2 as the oxidant, perhaps in the presence of better co-reductants than CO. Both DADLEC and LUSHOX04 have C-H activation barriers of 12 kcal/mol and 7 kcal/mol, respectively, suggesting that the relatively easily formed metal-oxo species can also activate the strong C-H bonds in methane (Figure and Supporting Information Figure ). Thus, the computed free energy landscapes show that DADLEC and LUSHOX04 have both favorable kinetics and thermodynamics for methane to methanol catalysis.