Mesoporous carbon and microporous zeolite supported Ru catalysts for selective levulinic acid hydrogenation into γ-valerolactone

Catalysis for Sustainable Energy Pub Date : 2019-01-01 DOI:10.1515/cse-2019-0004

I. Simakova, Y. Demidova, M. Simonov, P. Niphadkar, V. Bokade, N. Devi, P. Dhepe, D. Murzin

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引用次数: 9

Abstract

Abstract Ru supported on mesoporous carbon Sibunit and microporous zeolites (HZSM-5, SiO2/Al2O3 = 250; H-Beta, SiO2/Al2O3 = 30; H-Y, SiO2/Al2O3 = 5; H-USY, SiO2/Al2O3 = 30) synthesized by the sol-gel method (CSIR-National Chemical Laboratory, Pune India) were prepared by impregnation of the corresponding supports with RuCl3∙nH2O (0.1 M) followed by reduction in H2. Catalyst screening in levulinic acid (LA) (15 mL, 6.9 mmol) hydrogenation into g-valerolactone (GVL) with 1,4-dioxane (165°C, hydrogen pressure ca. 16 bar) as a solvent showed higher activity and selectivity to GVL of Ru/zeolites compared to carbon supported catalysts. Among Ru/zeolites LA conversion increased as follows Ru/HZSM-5 < Ru/H-Y < Ru/H-USY < Ru/H-Beta demonstrating a clear advantage of H-Beta preparation method. Optimization of the support microstructure and acidity opens a reliable way for selective catalytic LA hydrogenation to GVL. The catalysts were analyzed by TEM, XRD, H2-TPR and N2 physisorption to compare their physical chemical properties.

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介孔碳和微孔沸石负载Ru催化剂选择性乙酰丙酸加氢制备γ-戊内酯

Ru负载于介孔碳硅基和微孔沸石(HZSM-5, SiO2/Al2O3 = 250;h - β， SiO2/Al2O3 = 30;H-Y, SiO2/Al2O3 = 5;采用溶胶-凝胶法制备H-USY, SiO2/Al2O3 = 30 (CSIR-National Chemical Laboratory, Pune India)，将相应的载体用RuCl3∙nH2O (0.1 M)浸渍，再用H2还原。以1,4-二氧六环(165℃，氢压约16 bar)为溶剂，乙酰丙酸(LA) (15 mL, 6.9 mmol)加氢生成g-戊内酯(GVL)的催化剂筛选结果表明，与碳负载型催化剂相比，Ru/沸石的GVL活性和选择性更高。在Ru/分子筛中，LA转化率依次为Ru/HZSM-5 < Ru/H-Y < Ru/H-USY < Ru/H-Beta，表明了H-Beta制备方法的明显优势。通过对载体结构和酸度的优化，为LA选择性加氢制备GVL开辟了一条可靠的途径。采用TEM、XRD、H2-TPR、N2吸附等方法对催化剂进行了理化性能分析。

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Catalysis for Sustainable Energy

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