NDLI: UiO-66 derived Ru/ZrO<sub>2</sub>@C as a highly stable catalyst for hydrogenation of levulinic acid to γ-valerolactone

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UiO-66 derived Ru/ZrO₂@C as a highly stable catalyst for hydrogenation of levulinic acid to γ-valerolactone

Content Provider	Royal Society of Chemistry (RSC)
Author	Ge, Hongguang Luo, Wenhao Cao, Wenxiu Wang, Aiqin Su, Yang Zhang, Tao
Copyright Year	2017
Abstract	The hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) is a crucial reaction included in many biorefinery schemes for the production of renewable chemicals and fuels. The development of highly stable supported Ru-based catalysts in the polar protic liquid phase under hydrothermal conditions is still a major challenge. Here, we prepared a 0.85 wt% Ru/ZrO2@C catalyst using a new stabilization strategy based on the UiO-66 (Zr-MOF) material. The catalytic performance of this Ru/ZrO2@C in LA-to-GVL was tested and compared with commercial 5 wt% Ru/C at 10 bar H2, 413 K in water and also in high protic aqueous solution (pH = 1). The full conversion of LA and quantitative yield of GVL were achieved with both catalysts. However, the 5 wt% Ru/C showed poor resistance to deactivation already after the first run. ICP, XPS, HRTEM, AC-STEM, TPR and physisorption data showed that quick deactivation of Ru/C was mainly caused by the leaching of ruthenium in addition to the loss of surface area via carbonaceous deposition in micro-pores. In contrast, the self-prepared Ru/ZrO2@C catalyst showed no apparent drop in catalytic performance either in water or in high protic aqueous solution upon multiple recycling, and no leaching of ruthenium was found even under harsh conditions (pH = 1). Remarkably, in the Ru/ZrO2@C catalyst, Ru (probable single-atom) was highly dispersed on nanotetragonal ZrO2 (3.3 nm), embedded in the amorphous carbon, and no apparent Ru nanoclusters were observed even after reactions. TPR results indicated that this excellent stability might be attributed to strong metal–support interaction between Ru and nanotetragonal ZrO2.
Starting Page	2201
Ending Page	2211
Page Count	11
File Format	HTM / HTML PDF
ISSN	14639262
Volume Number	19
Issue Number	9
Journal	Green Chemistry
DOI	10.1039/c7gc00512a
Language	English
Publisher	Royal Society of Chemistry
Access Restriction	Open
Subject Keyword	TPR LA ICP Hydrogenation Carboxylic acid Los Angeles Gamma-Valerolactone Biorefinery Renewable energy Hydrothermal circulation Zirconium dioxide PH Physisorption Ruthenium Amorphous carbon
Content Type	Text
Resource Type	Article
Subject	Environmental Chemistry Pollution

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Efficient aqueous hydrogenation of levulinic acid to γ-valerolactone over a highly active and stable ruthenium catalyst

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UiO-66 derived Ru/ZrO₂@C as a highly stable catalyst for hydrogenation of levulinic acid to γ-valerolactone

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UiO-66 derived Ru/ZrO2@C as a highly stable catalyst for hydrogenation of levulinic acid to γ-valerolactone

UiO-66 derived Ru/ZrO₂@C as a highly stable catalyst for hydrogenation of levulinic acid to γ-valerolactone