Journal
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
Volume 8, Issue 1, Pages 393-402Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.9b05546
Keywords
lignocellulosic Biomass; levulinic Acid; formic Acid; mesoporous ZrO2; gamma-valerolactone; aqueous-phase hydrogenation
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Funding
- German Federal Ministry of Education and Research [03EK3508B]
- COST Action [FP1306]
- National Science Fund of Bulgaria [KPi-06-KOCT/3]
- Bulgarian Ministry of Education and Science under the National Research Programme E+: Low Carbon Energy for the Transport and Households [D01-2014/19.11.18]
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Monometallic Pt catalysts supported on mesoporous (MP) ZrO2 were prepared and utilized as catalysts in the aqueous-phase upgrading of lignocellulosic biomass-derived levulinic acid (LA), with formic acid (FA) serving as a sustainable reducing agent. Among the studied catalysts, 1.6Pt/mesoporous ZrO2 showed the highest LA conversion (97%) and a gamma-valerolactone (GVL) yield (90%) at 513 K after 24 h of reaction was achieved. This high LA conversion and GVL yield obtained can be attributed to the high specific surface area (204 m(2) g(-1)) and density of acid sites (136 mu mol g(-1)) and Pt dispersion (37%). Furthermore, this catalyst exhibits high stability after 96 h of reaction time, that is, four catalytic repetitions, with a GVL yield above 60% and no change in the crystal structure of the support. A high reaction temperature (533 K) tends to shift the reaction equilibrium from GVL to pentanoic acid which is formed with a yield of 22% after 24 h. Even after increasing the complexity of the model mixture by adding vanillin (V) as a lignin-derived model compound to the aqueous solution of LA and FA, the catalyst remained stable and the hydrogenation of LA and V succeeded, resulting in 43% of GVL and 65% of 2-methoxy-4-methylphenol after 24 h at 513 K.
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