Dataset Information

Influence of Levulinic Acid Hydrogenation on Aluminum Coordination in Zeolite-Supported Ruthenium Catalysts: A ²⁷ Al 3QMAS Nuclear Magnetic Resonance Study.

ABSTRACT: The influence of a highly oxygenated, polar protic reaction medium, that is, levulinic acid in 2-ethylhexanoic acid, on the dealumination of two zeolite-supported ruthenium catalysts, namely Ru/H-β and Ru/H-ZSM-5, has been investigated by ²⁷ Al triple-quantum magic-angle spinning nuclear magnetic resonance spectroscopy (3QMAS NMR). Upon use of these catalysts in the hydrogenation of levulinic acid, the heterogeneity in aluminum speciation is found to increase for both Ru/H-ZSM-5 and Ru/H-β. For Ru/H-ZSM-5, the symmetric, tetrahedral framework aluminum species (FAL) were found to be mainly converted into distorted tetrahedral FAL species, with limited loss of aluminum to the solution by leaching. A severe loss of both FAL and extra-framework aluminum (EFAL) species into the liquid phase was observed for Ru/H-β instead. The large decrease in tetrahedral FAL species, in particular, results in a significant decrease in strong acid sites, as corroborated by Fourier transform infrared spectroscopy (FT-IR). This decrease in acidity, evidence of the inferior stability of the strongly acidic sites in Ru/H-β relative to Ru/H-ZSM-5 under the applied conditions, is considered as the main reason for differences seen in catalyst performance.

SUBMITTER: Luo W

PROVIDER: S-EPMC5836955 | biostudies-literature | 2018 Feb

REPOSITORIES: biostudies-literature

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Influence of Levulinic Acid Hydrogenation on Aluminum Coordination in Zeolite-Supported Ruthenium Catalysts: A <sup>27</sup> Al 3QMAS Nuclear Magnetic Resonance Study.

Luo Wenhao W van Eck Ernst R H ERH Bruijnincx Pieter C A PCA Weckhuysen Bert M BM

Chemphyschem : a European journal of chemical physics and physical chemistry 20171122 4

The influence of a highly oxygenated, polar protic reaction medium, that is, levulinic acid in 2-ethylhexanoic acid, on the dealumination of two zeolite-supported ruthenium catalysts, namely Ru/H-β and Ru/H-ZSM-5, has been investigated by <sup>27</sup> Al triple-quantum magic-angle spinning nuclear magnetic resonance spectroscopy (3QMAS NMR). Upon use of these catalysts in the hydrogenation of levulinic acid, the heterogeneity in aluminum speciation is found to increase for both Ru/H-ZSM-5 and R ...[more]

PMID: 29164764

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Project description:Zeolites with different structures (P1, sodalite, and X) were synthesized from coal fly ash by applying ultrasonically assisted hydrothermal and fusion-hydrothermal synthesis. Bimetallic catalysts, containing 5 wt.% Ni and 2.5 wt.% Cu, supported on the zeolites, were prepared by a post-synthesis incipient wetness impregnation method. The catalysts were characterized by X-ray powder diffraction (XRPD), N2 physisorption, transmission electron microscopy (TEM), Mössbauer and X-ray photoelectron spectroscopies (XPS), and H2-temperature-programmed reduction (H2-TPR) analyses. The XRPD results showed that crystalline Cu0 and NixCuy intermetallic nanoparticles were formed in the reduced catalysts. The presence of the intermetallic phase affected the reducibility of the nickel by shifting it to a lower temperature, as confirmed by the H2-TPR curves. Based on the Mössbauer spectroscopic results, it was established that the iron contamination of the coal fly ash zeolites (CFAZs) was distributed in ionic positions of the zeolite lattice and as a finely dispersed iron oxide phase on the external surface of the supports. The formation of the NiFe alloy, not detectable by XRPD, was also evidenced on the impregnated samples. The catalysts were studied in the upgrading of levulinic acid (LA), derived from lignocellulosic biomass, to γ-valerolactone (GVL), in a batch reactor under 30 bar H2 pressure at 150 and 200 °C, applying water as a solvent. The NiCu/SOD and NiCu/X catalysts showed total LA conversion and a high GVL yield (>75%) at a reaction temperature of 200 °C. It was found that the textural parameters of the catalysts have less influence on the catalytic activity, but rather the stable dispersion of metals during the reaction. The characterization of the spent catalyst found the rearrangement of the support structure. The high LA conversion and GVL yield can be attributed to the weak acidic character of the support and the moderate hydrogenation activity of the Ni-Cu sites with high dispersion.

Dataset Information

Influence of Levulinic Acid Hydrogenation on Aluminum Coordination in Zeolite-Supported Ruthenium Catalysts: A ²⁷ Al 3QMAS Nuclear Magnetic Resonance Study.

Publications

Influence of Levulinic Acid Hydrogenation on Aluminum Coordination in Zeolite-Supported Ruthenium Catalysts: A <sup>27</sup> Al 3QMAS Nuclear Magnetic Resonance Study.

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Dataset Information

Influence of Levulinic Acid Hydrogenation on Aluminum Coordination in Zeolite-Supported Ruthenium Catalysts: A 27 Al 3QMAS Nuclear Magnetic Resonance Study.

Publications

Influence of Levulinic Acid Hydrogenation on Aluminum Coordination in Zeolite-Supported Ruthenium Catalysts: A <sup>27</sup> Al 3QMAS Nuclear Magnetic Resonance Study.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

Tweets

Influence of Levulinic Acid Hydrogenation on Aluminum Coordination in Zeolite-Supported Ruthenium Catalysts: A ²⁷ Al 3QMAS Nuclear Magnetic Resonance Study.