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We have established that bipyridinium radicals can be reversibly π‐dimerized under the combined effects of chemical (proton transfer) and electrochemical (electron transfer) stimuli. Our investigations also led to the discovery that a bis‐pyridinyl appended calixarene intermediate is involved in a fully reversible redox‐triggered σ‐dimerization process. The structure of the most stable intramolecular...
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