Sustainable Catalytic Synthesis for a Bio‐Based Alternative to the Reach‐Restricted N‐Methyl‐2‐Pyrrolidone

Abstract The catalytic conversion of biomass and its derivatives into valuable chemicals requires efficient, energy saving, and sustainable technologies. In this work, a variety of bifunctional catalysts are prepared combining immobilized metal nanoparticles and acid solid materials featuring Lewis or Brønsted acidity. The catalytic systems are tested in the reductive amination of bio‐derived levulinates with primary amines, using hydrogen as clean reducing agent, to obtain N‐substituted‐5‐methyl‐2‐pyrrolidones, which are proposed as substitutes for the widely used, REACH‐restricted solvent N‐methyl‐2‐pyrrolidone. The overall process is studied in depth to identify the best combination of metal and acid functionalities to be used in one‐pot and one stage. Pt immobilized onto the Brønsted solid acid Aquivion is shown to be the most efficient catalyst, with a productivity of N‐heptyl‐5‐methyl‐2‐pyrrolidone of 7.9 mmolg_cat⁻¹ h⁻¹ reached at full conversion and 98.6% selectivity, under 120 °C, 4 bar H₂ pressure and solvent‐free conditions.