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The mechanism of the copper‐catalyzed arylation of nitrogen heterocycles using anilines via diazonium salts has been studied by combining DFT and experimental data. A CuI/CuIII redox mechanism is proposed. Our study has revealed the multiple roles of the acid/base couple AcOH/AcO–. An in situ formed triazene species maintains a low concentration of diazonium salts in the reaction medium, which ensures...
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