Calculated useable surface coverages (Δθ) and gravimetric and volumetric O₂ working capacities for nine frameworks discussed in the text as implemented in VTSA process with P_ads = 0.21 bar O₂ at 298 K and P_des = 0.01 bar at 338 K. Gravimetric working capacities (mmol g⁻¹) were obtained by multiplying Δθ by estimated gravimetric O₂ capacities for each MOF, determined in most cases from the inflection point of the experimental isosteric heat of adsorption as a function of loading (see Section S5 of the ESI for details).^a Volumetric working capacities (g L⁻¹) were calculated by multiplying Δθ by the estimated volumetric O₂ capacity for each framework (see Table S12 for details).

MOF	Surface coverage, Δθ	Working capacity (mmol g−1)	Working capacity (g L−1)
Co-BTP	0.86	2.4	78.0
CuI-MFU-4l	0.71	1.1	20.3
Co-BDTriP	0.43	0.90	29.2
Mn-PCN-224	0.52	0.29	4.3
Co-BTTri	0.083	0.23	6.8
Fe-BTTri	0.095	0.22	6.2
Fe-PCN-224 HT	0.088	0.048	0.77
Co-PCN-224	0.068	0.048	0.75
Co2(OH)2(bbta)	0.014	0.035	1.2
Fe-PCN-224 LT	0.039	0.021	0.34

^aThe inflection point was approximated from the second derivative of the enthalpy versus loading, estimated using the finite difference method.