For an efficient capture-and-release process that makes use of a spin crossover-induced gas-release, two conditions are necessary: i) a large change in binding energy upon spin crossover and ii) a transition temperature close to the adsorption condition. In this section we compute the binding configuration and binding energy for each spin state and the corresponding adiabatic energy difference in metalorganic frameworks exhibiting the open-metal site coordination studied in the previous section. We have found that the predicted changes in binding energy are substantial when the occupation of the d z 2 changes and this may lead to efficient gas release, depending on the thermodynamics of the transition. We recall that for Ni(II), HS results in a stronger interaction with the gas because the d z 2 is singly occupied while it is doubly occupied in LS. Thus, in this case gas Because the open metal site exhibit a divalent metal, here M=Fe(II), Ni(II), and Mn(II). The latter is isoelectronic to (and replaces) Fe(III). We note that the Ni case has been largely studied experimentally for both bpac and pz. In each case we compute the ground state and the first accessible state. This corresponds to S=0 and S=1 for Fe(II) and Ni(II), and S=1/2 and S=3/2 for Mn(II).