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A giant organometallic molecule and a 2D coordination polymer are formed by template‐assisted self‐assembly between CuCl and the cyclo‐P5 complex [Cp*Fe(η5‐P5)]. The giant capsular molecule exhibits a skeleton of 110 inorganic core atoms and consists of two half‐shells with threefold symmetry. Dipersion forces between two encapsulated [Cp*Fe(η5‐P5)] guest complexes and half‐shells are responsible...
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