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The only operating mechanism in the oxidation of water to dioxygen catalyzed by the mononuclear cis‐[RuII(bpy)2(H2O)2]2+ complex when treated with excess CeIV was unambiguously established. Theoretical calculations together with 18O‐labeling experiments (see plot) revealed that it is the nucleophilic attack of water on a RuO group.
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