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A Cu–MOF-catalyzed C–H functionalization of substituted amidines was developed for the facile and efficient synthesis of benzimidazoles. More importantly, this transformation is compatible with various substrates derived from aryl nitriles without ortho substituents. Under reaction conditions devoid of O2 atmosphere or specific groups, 537-MOF has been revealed as a key parameter for expanding the reaction scope and increasing the yield up to 96%. Importantly, this strategy also provides numerous opportunities for further utilization of MOFs as catalysts for challenging organic reactions.

Synergic effect of copper-based metal–organic frameworks for highly efficient C–H activation of amidines