Continuous hydrogenation of aqueous levulinic acid to γ-valerolactone under mild conditions with a highly efficient multifunctional Ru/carbon catalyst
2025 (English)In: Applied Catalysis A: General, ISSN 0926-860X, E-ISSN 1873-3875, Vol. 706, article id 120494Article in journal (Refereed) Published
Abstract [en]
Herein, a Ru-decorated carbon material bearing unique surface chemistry (Brønsted acidic phosphate groups, Lewis basic N-groups and oxygen functional groups) is shown to exhibit exceptional activity, selectivity and stability upon direct hydrogenation of aqueous levulinic acid (LA) (0.47 M and 0.95 M) to γ-valerolactone (GVL) under mild conditions (25–95 °C and 3.5–5 bar). The multifunctional Ru/carbon catalyst outperformed the bifunctional Ru/NbOPO4, and blended (physically mixed) catalytic systems comprising of commercial Ru/carbon (hydrogenation catalyst) and NbOPO4/Amberlyst 15 (acid promoter/co-catalyst). The material also demonstrated remarkable stability for energy efficient GVL production in a fixed-bed reactor under continuous flow conditions, maintaining stable GVL productivity during 52-day time on stream operating at 3.5–5 bar, 80–95 °C and low H2/LA ratio (4–17:1 mol/mol). The exceptional catalytic performance and long term stability of the multifunctional carbocatalyst was attributed to the presence of highly active Ru(0) nanoparticles stabilized on N-doped carbon framework and acidic phosphates and RuOx/RuO2 sites, which promote LA hydrogenation and intramolecular esterification of 4-hydroxypenatonnic (4-HPA) in tandem, affording a high GVL selectivity. The catalyst's combination of high productivity, long-term stability, and ability work under intensified setting in mid conditions highlight its potential for energy efficient GVL production at large scale.
Place, publisher, year, edition, pages
Elsevier, 2025. Vol. 706, article id 120494
Keywords [en]
Levulinic acid, Multifunctional catalysts, Ru-based catalysts, Selective hydrogenation, γ-valerolactone
National Category
Organic Chemistry
Identifiers
URN: urn:nbn:se:umu:diva-243065DOI: 10.1016/j.apcata.2025.120494Scopus ID: 2-s2.0-105012596149OAI: oai:DiVA.org:umu-243065DiVA, id: diva2:1994095
Funder
Bio4EnergyThe Kempe Foundations2025-09-022025-09-022025-09-02Bibliographically approved