Synergy of ultra-low-loaded ruthenium with alumina stimulating the catalytic hydrogenation of levulinic acid into γ-valerolactone

Liu, Zhenzhen; Gao, Xueying; Song, Guoyong

doi:10.1016/j.cej.2023.143869

Cited by 13 publications

(3 citation statements)

References 62 publications

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“…The data suggest that 0.25% Pd/Nb 2 O 5 can efficiently cleave the C–OH bonds of gluconic acid to produce mainly levulinic acid (a keto acid), carboxylic acids, and cyclic ketones. The levulinic acid undergoes dehydration and hydrogenation on metal–acid sites to form GVL, 70 while the gluconic acid lactones were formed via the cyclization of gluconic acid. 19 We further compared the niobia-supported metal catalysts with carbon-supported metals at the same conditions (i.e., low conversion), and the results are shown in Figure S16 .…”

Section: Resultsmentioning

confidence: 99%

Catalytic Upgrading of a Mixed Hydroxy Acid Feedstock Derived from Kraft Black Liquor

Ojelade,

Fu,

Nair

et al. 2024

ACS Sustainable Chem. Eng.

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Lignocellulosic feedstocks are widely studied for sustainable liquid fuel and chemical production. The pulp and paper industry generates large amounts of kraft black liquor (BL) from which a high volume of hydroxy acids (HAs) can be separated for further catalytic processing. Here, we explore the catalytic upgrading of HAs, including the conversion of (1) a model HA, gluconic acid; (2) a model mixture of HAs, and (3) a real mixture of HAs derived from kraft BL on M/Nb2O5 (M = Pd, Pt, Rh, and Ru). The hydrodeoxygenation of model gluconic acid reveals that “volatile” carboxylic acids (mainly C2 and C3), levulinic acid, and cyclic esters are significant products over all the catalysts, with Pd/Nb2O5 showing superior activity and selectivity toward valuable intermediates. The model mixture of HAs shows a wide range of reactivity over the supported metal catalyst, with the product selectivity strongly correlating to reaction temperature. Utilizing a 0.25% Pd/Nb2O5 catalyst, a real mixture of HAs derived from kraft BL is successfully dehydroxylated to produce a mixture rich in C3–C8 carboxylic acids that may be amenable for further upgrading, e.g., catalytically to ketones with high carbon chain lengths. Despite the feedstock complexity, we selectively cleaved the C–OH bonds of HAs, while successfully preserving most of the −COOH groups and minimizing C–C and CO bond scission reactions under the operating conditions tested. The BL-derived HA stream is thus proposed to be a suitable platform for producing mixed carboxylic acid products from an overoxygenated byproduct feed.

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Section: Resultsmentioning

confidence: 99%

Catalytic Upgrading of a Mixed Hydroxy Acid Feedstock Derived from Kraft Black Liquor

Ojelade,

Fu,

Nair

et al. 2024

ACS Sustainable Chem. Eng.

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“…Heterogeneous catalysts, i.e. , Ru-, 9–14 Pt-, 15 Fe-, 16 Co-, 17 Ni-, 18 and Cu-based catalysts, 16,19 exhibit good activity for LA hydrogenation. Compared with heterogeneous catalysts, homogeneous catalysts, including Ru-, 20–24 Ir-, 25–27 Pt-, 28 and Ni-containing complexes, 5,29 have higher catalytic efficiency and selectivity under mild reaction conditions.…”

Section: Introductionmentioning

confidence: 99%

Mechanism of CO₂ in promoting the hydrogenation of levulinic acid to γ-valerolactone catalyzed by RuCl₃ in aqueous solution

Min,

Xiong,

Liu

et al. 2024

Phys. Chem. Chem. Phys.

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“…[12] Among the investigated noble metal catalysts, such as Ru, Ir, Pd, Rh, and Pt, ruthenium-based catalysts have an extremely excellent catalytic ability to convert LA to GVL under solventfree conditions. [13][14] Non-noble metal catalysts represented by Ni, Cu, and Co are more competitive in the solvent-free hydrogenation of LA to GVL because of the price limitation of the precious metal catalysts. [15] The metal Ni has strong ability for the hydrogenation of LA but weak selectivity for the generation of GVL, whereas the metal Cu can inhibit the decomposition of LA during the reaction.…”

Section: Introductionmentioning

confidence: 99%

Solvent‐Free Efficient Hydrogenation of Levulinic Acid over Silicotungstic Acid Promoting the Activity of CuNiAl Catalysts: A Synergistic Effect

Wei,

Shao,

Wang

et al. 2024

ChemistrySelect

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Multi‐metallic catalysts rely on the synergistic effect between metals to perform better catalytic effect in biomass hydrogenation experiments compared with mono‐metallic catalysts. A series of CuNiAl composite metal oxide catalysts promoted by silicotungstic acid (HSiW), which were prepared by co‐precipitation and impregnation methods, were characterized by powder X‐ray diffraction (XRD), N2‐physisorption, scanning electron microscope (SEM) and NH3 program temperature desorption (NH3‐TPD) and pyridine infrared adsorption (Py‐FTIR). Their catalytic performance was evaluated in the hydrogenation of levulinic acid (LA) to prepare γ‐valerolactone (GVL). The results showed that the addition of Cu could improve the hydrogenation activity of Ni, and the addition of HSiW could further increase the amount of acid sites in the catalysts. Both of them could enhance the conversion of LA to some extent. CuNiAl‐5SiW, the par excellence catalyst, relied on the synergistic interactions between metals as well as the Brønsted and Lewis acid active sites to show efficient hydrogenation performance. The CuNiAl‐5SiW catalyst demonstrated 96.9 % conversion of LA and more than 99 % selectivity to GVL under 2 hours of reaction time, 180 °C of reaction temperature, 3.0 MPa of initial hydrogen pressure and solvent‐free conditions.

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Synergy of ultra-low-loaded ruthenium with alumina stimulating the catalytic hydrogenation of levulinic acid into γ-valerolactone

Cited by 13 publications

References 62 publications

Catalytic Upgrading of a Mixed Hydroxy Acid Feedstock Derived from Kraft Black Liquor

Catalytic Upgrading of a Mixed Hydroxy Acid Feedstock Derived from Kraft Black Liquor

Mechanism of CO₂ in promoting the hydrogenation of levulinic acid to γ-valerolactone catalyzed by RuCl₃ in aqueous solution

Solvent‐Free Efficient Hydrogenation of Levulinic Acid over Silicotungstic Acid Promoting the Activity of CuNiAl Catalysts: A Synergistic Effect

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Synergy of ultra-low-loaded ruthenium with alumina stimulating the catalytic hydrogenation of levulinic acid into γ-valerolactone

Cited by 13 publications

References 62 publications

Catalytic Upgrading of a Mixed Hydroxy Acid Feedstock Derived from Kraft Black Liquor

Catalytic Upgrading of a Mixed Hydroxy Acid Feedstock Derived from Kraft Black Liquor

Mechanism of CO2 in promoting the hydrogenation of levulinic acid to γ-valerolactone catalyzed by RuCl3 in aqueous solution

Solvent‐Free Efficient Hydrogenation of Levulinic Acid over Silicotungstic Acid Promoting the Activity of CuNiAl Catalysts: A Synergistic Effect

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Mechanism of CO₂ in promoting the hydrogenation of levulinic acid to γ-valerolactone catalyzed by RuCl₃ in aqueous solution