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Pentaphosphaferrocenes [CpRFe(η5‐P5)] (Cp*=η5‐C5Me5) (A), Cp’’=η5‐C5H3tBu2‐1,3 (B)) are excellent building blocks for polymeric assemblies in supramolecular chemistry in combination with coinage metal salts of weakly coordinating anions such as AgSbF6. Adding rigid aromatic dinitriles ortho/meta/para‐(NC)2C6H4 in a one‐pot reaction between [CpRFe(η5‐P5)] and AgSbF6 leads to various coordination polymers...
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