Abstract

This study reports one of the few examples of acylhydrazide synthesis catalyzed by the metal–organic framework (MOF) MIL-53(Al) via the aldehyde C(sp2)–H hydrazidation reaction. The material exhibited high catalytic performance, displaying a broad substrate scope and affording yields of up to 97%. The catalyst retained its structural integrity and activity for at least four consecutive cycles, with no significant metal leaching. Notably, MIL-53(Al) was synthesized from waste-derived materials and thoroughly characterized to confirm its crystallinity, structural integrity, and porosity – features essential to its catalytic function. This work demonstrates the potential of upcycled MIL-53(Al) as a stable, sustainable, and low-cost heterogeneous catalyst for the synthesis of valuable acylhydrazides, offering an attractive alternative to conventional systems that rely on toxic metal promoters. This journal is © The Royal Society of Chemistry, 2025