Direct Mechanoorganocatalysis via Surface Functionalization of Milling Reactors With Amine Functions

Mechanochemistry via ball milling offers a sustainable alternative to solution‐based synthesis, yet direct organocatalysis under these conditions remains unexplored. Here we report epoxy resin milling jars functionalized with piperazine, enabling efficient direct mechanoorganocatalysis. These reusable jars catalyzed Knoevenagel condensations and multicomponent reactions under solvent‐free conditions, achieving high conversions and yields with simplified product isolation. The catalytic surface remained active over multiple cycles, with no evidence for significant leaching or contamination. This approach demonstrates a practical strategy for immobilizing organocatalysts on milling reactor surfaces, advancing sustainable mechanochemical synthesis by combining catalyst recovery, efficiency, and operational simplicity.