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The light‐driven reduction of protons for the production of molecular hydrogen in multicomponent systems depends on electron relays such as viologens. We describe here the effect of viologens appended with guest moieties (adamantane or bile acid) on the efficiency of a system composed of a cyclodextrin‐appended photosensitizer [Ir(ppy)2(pytl‐βCD)]Cl [ppy = 2‐phenylpyridine; pytl = 2‐(1‐substituted‐1...
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