A Two-Dimensional Spin-Crossover Coordination Polymer Exhibiting Interlayer Multiple C–Hδ+···Hδ−–B Dihydrogen Bonds

The reaction of 1,1,2,2-tetrakis(4-(pyridin-4-yl)phenyl)ethene (tppe) with [Fe(NCBH 3 ) 2 ] produced a two-dimensional coordination polymer [Fe(NCBH 3 ) 2 (tppe)] n ( 1 ), which was pillared in an ABAB manner through interlayer multiple [C–H δ+ ···H δ− –B] dihydrogen bonds (DHBs) to form a stable porous three-dimensional (3D) supramolecular structure that showed guest-molecule-dependent spin-crossover behaviors.