Despite the potentially high impact of this mechanism on the development of efficient capture technologies, the proofof-concept of this idea is still lacking possibly owing to the fact that its thermodynamic feasibility relies upon the delicate competition between the ligand field strength of the MOF linkers and that of the adsorbate. Ab initio electronic structure calculations are a critical ingredient towards such development. Thus, the well known challenge in computing the energy difference between different spin states (adiabatic energy difference) in periodic systems and with chemical accuracy has possibly hampered the development of this field.