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A stepwise self‐assembly protocol has been used to synthesize [2]‐ and [3]catenanes. Firstly, binuclear Cp*Rh/Ir‐directed (Cp*=pentamethylcyclopentadienyl) pseudorotaxanes were prepared through self‐assembly, driven by donor–acceptor interactions between electron‐deficient naphthalenediimide (NDI) units and an electron‐rich crown ether. Subsequently, the pre‐organized pseudorotaxanes were applied...
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