Jump to main content
Jump to site search
PLANNED MAINTENANCE Close the message box

Scheduled maintenance upgrade on Thursday 4th of May 2017 from 8.00am to 9.00am (BST).

During this time our websites will be offline temporarily. If you have any questions please use the feedback button on this page. We apologise for any inconvenience this might cause and thank you for your patience.



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

Author affiliations

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.

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

Back to tab navigation
Please wait while Download options loads

Supplementary files

Publication details

The article was received on 16 Feb 2017, accepted on 24 Mar 2017 and first published on 28 Mar 2017


Article type: Paper
DOI: 10.1039/C7GC00512A
Citation: Green Chem., 2017, Advance Article
  •   Request permissions

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

    W. Cao, W. Luo, H. Ge, Y. Su, A. Wang and T. Zhang, Green Chem., 2017, Advance Article , DOI: 10.1039/C7GC00512A

Search articles by author