Abstract
Reversible switching between the closed cyclic dimeric assembly [Cu2(1)2]2+ (OFF state) and the extended dimeric homoleptic complex [FeCu2(1)2]4+ (ON State) by addition/removal of Fe2+ triggered catalysis of a double‐click reaction and high yield preparation of [2]rotaxanes. Mechanistic and computational studies provide valuable general insight for double‐click strategies by revealing cooperative effects in the second cycloaddition step due to a distance‐tolerant preorganization of the first‐click product by the two copper(I)‐loaded phenanthroline subunits of [FeCu2(1)2]4+.
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