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Low temperature conversion of levulinic acid into γ-valerolactone using Zn to generate hydrogen from water and nickel catalysts supported on sepiolite.

ABSTRACT: In the present article, γ-valerolactone has been obtained from levulinic acid with a yield exceeding 25% using very mild conditions without feeding hydrogen (30 °C, atmospheric pressure, water as the hydrogen source). The overall reaction conducted is a two-step process: first, a redox reaction involving the oxidation of metallic Zn to ZnO for in situ hydrogen production through the water splitting reaction and, second, a catalytic reaction involving Ni-supported catalysts for the production of γ-valerolactone from levulinic acid. Ni active sites have been supported on sepiolite, an abundant and cheap material. The nickel particle size has been demonstrated to be a parameter of paramount importance determining the catalytic activity, since the best catalytic performance is obtained with the smallest Ni nanoparticles. This combination of Zn and Ni supported on sepiolite shows a good catalytic stability after three catalytic runs.

SUBMITTER: Garcia A

PROVIDER: S-EPMC9054250 | biostudies-literature | 2020 May

REPOSITORIES: biostudies-literature

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Low temperature conversion of levulinic acid into γ-valerolactone using Zn to generate hydrogen from water and nickel catalysts supported on sepiolite.

García Adrián A Sanchis Rut R Miguel Pablo J PJ Dejoz Ana M AM Pico María Pilar MP López María Luisa ML Álvarez-Serrano Inmaculada I García Tomás T Solsona Benjamín B

RSC advances 20200527 35

In the present article, γ-valerolactone has been obtained from levulinic acid with a yield exceeding 25% using very mild conditions without feeding hydrogen (30 °C, atmospheric pressure, water as the hydrogen source). The overall reaction conducted is a two-step process: first, a redox reaction involving the oxidation of metallic Zn to ZnO for <i>in situ</i> hydrogen production through the water splitting reaction and, second, a catalytic reaction involving Ni-supported catalysts for the product ...[more]

PMID: 35517762

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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

Low temperature conversion of levulinic acid into γ-valerolactone using Zn to generate hydrogen from water and nickel catalysts supported on sepiolite.

Publications

Low temperature conversion of levulinic acid into γ-valerolactone using Zn to generate hydrogen from water and nickel catalysts supported on sepiolite.

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