Hydrogen spillover on Ni@Graphene enables robust and efficient catalytic hydrogenation of aqueous levulinic acid to γ-valerolactone

• Published in: Applied catalysis. B, Environmental Vol. 361; p. 124595
• Main Authors: Zhang, Yuansen, Li, Yu, Shen, Chenyang, Yang, Chenyu, Wu, Hangzhi, Jiang, Congyan, Chen, Shanyong, Li, Muhong, Li, Yongting, Ding, Weiping, Guo, Xuefeng
• Format: Journal Article
• Language: English
• Published: Elsevier B.V 01.02.2025
• Subjects: Aqueous hydrogenation; Graphene encapsuled Ni catalyst; Hydrogen spillover; Levulinic acid; γ-Valerolactone; Levulinic acid; Graphene encapsuled Ni catalyst; Aqueous hydrogenation; Hydrogen spillover; γ-Valerolactone
• ISSN: 0926-3373
• DOI: 10.1016/j.apcatb.2024.124595

Hydrogenation of biomass-derived aqueous levulinic acid (LA) to produce γ-valerolactone (GVL) is a promising approach from biomass to sustainable platform chemicals. However, the practical application of this method is limited because aqueous LA is highly corrosive to metal-based hydrogenation catalyst in high-temperature hydrothermal environments. Herein, we encapsulated metallic Ni0 particles with a few layers of graphene using a hydrothermal carbon coating method to obtain Ni@FLG-600 catalyst, which exhibited efficient catalytic activity and excellent cycling stability for the hydrogenation of aqueous LA to GVL. The defect-rich graphene shell prevents the Ni0 from acid corrosion meanwhile selectively permits the passage of small H2 molecules. The resulted active H* on Ni0 spills over to the outer surface of graphene shell and reacts with LA. Remarkably, the amount of H* on graphene shell can be the descriptor of activity. This finding presents a new strategy for the fabrication of acid-resistant catalysts for aqueous biomass hydrogenation. [Display omitted] •Ni@FLG-600 is synthesized for aqueous hydrogenation of LA to GVL.•Ni0 encapsulated in a few layers of graphene is hydrothermally stable.•The Ni@FLG-600 catalyst can be reused twenty times without deactivation.•H2 passes through the defects in the graphene shell and is activated to H* on Ni0.•H* spills over to the graphene surface to react with LA.