The series of 2D solids, Fe(3XPy)₂[Fe(CN)₅NO] with 3X = 3-Fluoro, 3-Chloro, 3-Bromo, 3-Iodo and Py = Pyridine, was obtained by intercalation of the organic molecule (3XPy) between neighboring layers of 2D ferrous nitroprusside. The organic ligand was found coordinated to the axial positions for the iron atom linked at the equatorial N ends of the CN groups in the nitroprusside building block, [Fe(CN)₅NO]. The axial CN and NO ligands remain unlinked and contribute to the solid stability through attractive dipole-dipole interactions. The formed hybrid solids preserve the 2D nature because no chemical bond is established between neighboring organic molecules in the interlayer region. For X = F, a thermal induced spin transition was observed, but not for the remaining derivatives. The nature of such behavior is discussed according to the recorded XRD, Raman and Mössbauer data and computational calculations. The spin crossover transition in Fe(3FPy)₂[Fe(CN)₅NO] is an incomplete process, a sample fraction of about 50% remains in paramagnetic state, even at 5 K. The spin transition is accompanied of an atypical small structural change, corresponding to a variation of 0.7% for the unit cell volume. Such behavior finds explanation in both, the bonding properties of the N end of the CN ligands in the nitroprusside pseudo-octahedral block, and in the intermolecular interactions in the interlayer region.

通过插入有机分子，获得了一系列2D固体Fe（3XPy）₂ [Fe（CN）₅ NO]，其中3X = 3-氟，3-氯，3-溴，3-碘和Py =吡啶（3XPy）在相邻的2D亚铁硝普钠的相邻层之间。发现有机配体与在硝普钠结构单元[Fe（CN）₅中，CN基的赤道N端连接的铁原子的轴向位置协调没有]。轴向CN和NO配体保持未连接状态，并通过有吸引力的偶极-偶极相互作用促进了固体稳定性。形成的杂化固体保留了2D性质，因为在夹层区域中相邻的有机分子之间没有建立化学键。对于X = F，观察到热诱导的自旋跃迁，但对于其余的导数则没有。根据记录的XRD，拉曼和莫斯鲍尔数据和计算结果，讨论了这种行为的性质。Fe（3FPy）₂ [Fe（CN）₅NO]是一个不完全的过程，即使在5 K时，顺磁性也保持约50％的样品分数。自旋转变伴随着非典型的小结构变化，对应于单位晶胞体积的0.7％变化。这种现象在硝普钠伪八面体嵌段中CN配体的N端的键合性质以及层间区域中的分子间相互作用中均可找到解释。