The formation of amorphous Cu–MOF‐74 from crystalline Cu–MOF‐74 at 120 °C under strong alkali condition was reported for the first time, and it could be employed as an efficient heterogeneous catalyst for catalyzing cross‐coupling reactions between (hetero)aryl iodides/bromides and N‐H heterocycles in high yields. The solid catalyst showed high catalytic activity with minimal copper leaching in reaction solution and lower copper contamination in N‐arylated product than with other common copper/ligand systems, and it could be reused at least six times with no significant decrease in activity.
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