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New three-dimensional spin crossover (SCO) coordination polymers systematically constructed by the novel building unit [Ag I  2 (CN) 3 ], Fe II (3-Br-5-CH 3 pyridine) 2 [Ag I  2 (CN) 3 ][Ag I (CN) 2 ] ( 1 ), Fe II (3-Br-5-Clpyridine) 2 [Ag I  2 (CN) 3 ][Ag I (CN) 2 ] ( 2 ), and Fe II (3,5-Brpyridine) 2 [Ag I  2 (CN) 3 ][Ag I (CN) 2 ] ( 3 ), have been synthesized and characterized. The bismonodentate binuclear [Ag 2 (CN) 3 ] - and mononuclear [Ag I (CN) 2 ] - units and Fe II atoms assemble to form a 3D network structure. The structures of 1 - 3 are crystallographically identical, which made up the triply interpenetration combined with complicated intermolecular interactions including Ag···Ag, Ag···X (pyridine substituents) and π-stacking interactions. Magnetic and differential scanning calorimetry studies were performed for 1 - 3 . These compounds display a similar SCO behavior, while the critical temperatures ( T  c ) are shifted by the substituent effect. Due to the identical structures of 1 - 3 , the order of T  c clearly corresponds with the Hammett constant.

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A New Systematic Construction of Novel Three-Dimensional Spin Crossover Coordination Polymers Based on the [AgI2(CN)3] Building Unit