From Metal Powder to Super Catalyst: One‐Pot Transformation of Cu 0 Powder to MOF Embedded Nanoparticles for Multifunctional Catalysis

Comprehensive Summary Cu‐BTC (BTC = 1,3,5‐benzenetricarboxylic acid) framework faces environmental and scalability challenges in conventional synthesis due to energy‐intensive processes, using toxic solvents and costly precursors, with nanoparticle integration further complicating production through multi‐step procedures that degrade structural integrity. This study developed an innovative ambient‐temperature synthesis of Cu‐N coordinated Cu‐BTC MOF containing dispersed Cu/Cu₂O nanoparticles using economical Cu 0 powder. The N‐ligand‐mediated oxidation and deprotonation simultaneously achieve: (1) incorporation of 5 nm nanoparticles, (2) in situ formation of catalytic Cu–N bonds, and (3) manifestation of multifunctional catalytic performance. The Cu/Cu₂O@Cu‐BTC/N composite demonstrates outstanding catalytic activity, achieving high yields across multiple reactions: 91% in Knoevenagel condensation, 89% in Sonogashira coupling, 99% in Ullmann‐type C–N coupling, and 97% in indole C2‐acylation, along with exceptional photocatalytic hydrogen evolution performance (7.06 mmol·g –1 ·h –1 ). Notably, the synthetic protocol demonstrates excellent scalability, maintaining 90% yield at both 1 g and 10 g scales, thereby establishing a sustainable pathway for large‐scale production of multifunctional MOF catalysts with promising applications in green chemistry and energy‐related fields.