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Continuous hydrogenation of aqueous levulinic acid to γ-valerolactone under mild conditions with a highly efficient multifunctional Ru/carbon catalyst
Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen.
Umeå universitet, Teknisk-naturvetenskapliga fakulteten, Kemiska institutionen. Laboratory of Industrial Chemistry and Reaction Engineering, Johan Gadolin Process Chemistry Centre, Åbo Akademi University, Åbo-Turku, Finland.
2025 (Engelska)Ingår i: Applied Catalysis A: General, ISSN 0926-860X, E-ISSN 1873-3875, Vol. 706, artikel-id 120494Artikel i tidskrift (Refereegranskat) 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.

Ort, förlag, år, upplaga, sidor
Elsevier, 2025. Vol. 706, artikel-id 120494
Nyckelord [en]
Levulinic acid, Multifunctional catalysts, Ru-based catalysts, Selective hydrogenation, γ-valerolactone
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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
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Bio4EnergyKempestiftelsernaTillgänglig från: 2025-09-02 Skapad: 2025-09-02 Senast uppdaterad: 2025-09-02Bibliografiskt granskad

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Konwar, Lakhya JyotiSamikannu, AjaikumarMikkola, Jyri-Pekka

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