For every functional group X in Fig. , we begin with a "fresh" prepared Ni(PyC) 2 structure and carry out this in silico H Ñ X substitution procedure on each of its eight PyC ligands. This gives us a library of crude {Ni(PyC-o-X) 2 , Ni(PyC-m-X) 2 } crystal structure models. By construction, each Ni(PyC-X) 2 structure in the library inherits (i) the two-fold interpenetrated diamondoid network topology (see