Conversion of Cellulose to γ-Valerolactone over Raney Ni Catalyst Using H2O as a Hydrogen Source

The sustainable valorization of lignocellulosic biomass into high-value platform chemicals presents a crucial pathway for reducing reliance on fossil resources. Gamma (γ)-valerolactone (GVL) has gained recognition as a versatile bio-derived compound with broad applications in renewable energy systems and green chemical synthesis. While conventional GVL production strategies from carbohydrate biomass typically depend on noble metal catalysts paired with high-pressure hydrogen gas, these approaches face substantial technical barriers including catalyst costs, hydrogen storage requirements, and operational safety concerns in large-scale applications. This work develops an innovative catalytic system utilizing earth-abundant iron for in situ hydrogen generation through water splitting, integrated with Raney Ni as the hydrogenation catalyst. The designed two-stage process enables direct conversion of cellulose—first through acid hydrolysis to levulinic acid (LA) followed by catalytic hydrogenation to GVL without intermediate purification. Through systematic parameter optimization, a remarkable 61.9% overall GVL yield from cellulose feedstock was achieved. Furthermore, the methodology’s versatility was demonstrated through wheat straw conversion experiments, yielding 24.6% GVL. This integrated methodology explores a technically feasible pathway for direct cellulose-to-GVL conversion utilizing abundant water as the hydrogen source, effectively overcoming the critical limitations associated with conventional hydrogenation technologies regarding hydrogen infrastructure and process safety.