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Efficient Vapor-Phase Selective Hydrogenolysis of Bio-Levulinic Acid to γ-Valerolactone Using Cu Supported on Hydrotalcite Catalysts.

ABSTRACT: In this work, Cu nanoparticles (Cu NPs, 2-20 nm) supported on Hydrotalcite catalysts exhibit enhanced selectivity for γ-valerolactone (GVL) during hydrogenolysis of levulinic acid (LA). At 260 °C, over 3 wt% Cu achieved 87.5% of LA conversion with a maximum GVL selectivity (95%). In contrast, LA hydrogenolysis over 3Cu/Hydrotalcite catalyst is highly active and stable toward the production of GVL due to balanced acido-basicity and higher Cu dispersion with ultrasmall particle sizes, which are investigated through the temperature programmed desorption (TPD) of ammonia, N₂O titration, and transmission electron microscopy (TEM) analysis. Hydrotalcite in combination with inexpensive Cu catalyst is found to be an efficient and environmentally benign for LA hydrogenolysis.

SUBMITTER: Mitta H

PROVIDER: S-EPMC6360448 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Robust Ruthenium Catalysts Supported on Mesoporous Cyclodextrin-Templated TiO2-SiO2 Mixed Oxides for the Hydrogenation of Levulinic Acid to γ-Valerolactone.

Project description:In this paper, we present a versatile template-directed colloidal self-assembly method for the fabrication in aqueous phase of composition-tuned mesoporous RuO2@TiO2-SiO2 catalysts. Randomly methylated β-cyclodextrin/Pluronic F127 supramolecular assemblies were used as soft templates, TiO2 colloids as building blocks, and tetraethyl orthosilicate as a silica source. Catalysts were characterized at different stages of their synthesis using dynamic light scattering, N2-adsorption analysis, powder X-ray diffraction, temperature programmed reduction, high-resolution transmission electron microscopy, high-angle annular bright-field and dark-field scanning transmission electron microscopy, together with EDS elemental mapping. Results revealed that both the supramolecular template and the silica loading had a strong impact on the pore characteristics and crystalline structure of the mixed oxides, as well as on the morphology of the RuO2 nanocrystals. Their catalytic performance was then evaluated in the aqueous phase hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) under mild conditions (50 °C, 50 bar H2). Results showed that the cyclodextrin-derived catalyst displayed almost quantitative LA conversion and 99% GVL yield in less than one hour. Moreover, this catalyst could be reused at least five times without loss of activity. This work offers an effective approach to the utilization of cyclodextrins for engineering the surface morphology of Ru nanocrystals and pore characteristics of TiO2-based materials for catalytic applications in hydrogenation reactions.

| S-EPMC7915766 | biostudies-literature

Nanostructured Nickel/Silica Catalysts for Continuous Flow Conversion of Levulinic Acid to γ-Valerolactone.

Project description:Selective transformation of levulinic acid (LA) to γ-valerolactone (GVL) using novel heterogeneous catalysts is one of the promising strategies for viable biomass processing. In this framework, we developed a continuous flow process for the selective hydrogenation of LA to GVL using several nanostructured Ni/SiO2 catalysts. The structural, textural, acidic, and redox properties of Ni/SiO2 catalysts, tuned by selectively varying the Ni amount from 5 to 40 wt %, were critically investigated using numerous materials characterization techniques. Electron microscopy images showed the formation of uniformly dispersed Ni nanoparticles on the SiO2 support, up to 30% Ni loading (average particle size is 9.2 nm), followed by a drastic increase in the particles size (21.3 nm) for 40% Ni-loaded catalyst. The fine dispersion of Ni particles has elicited a synergistic metal-support interaction, especially in 30% Ni/SiO2 catalyst, resulting in enhanced acidic and redox properties. Among the various catalysts tested, the 30% Ni/SiO2 catalyst showed the best performance with a remarkable 98% selectivity of GVL at complete conversion of LA for 2 h reaction time. Interestingly, this catalyst showed a steady selectivity to GVL (>97%), with a 54.5% conversion of LA during 20 h time-on-stream. The best performance of 30% Ni/SiO2 catalyst was attributed to well-balanced catalytic properties, such as ample amounts of strong acidic sites and abundant active metal sites. The obtained results show a great potential of applying earth-abundant nickel/silica catalysts for upgrading biomass platform molecules into value-added chemicals and high-energy-density fuels.

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High performing and stable supported nano-alloys for the catalytic hydrogenation of levulinic acid to ?-valerolactone.

Project description:The catalytic hydrogenation of levulinic acid, a key platform molecule in many biorefinery schemes, into ?-valerolactone is considered as one of the pivotal reactions to convert lignocellulose-based biomass into renewable fuels and chemicals. Here we report on the development of highly active, selective and stable supported metal catalysts for this reaction and on the beneficial effects of metal nano-alloying. Bimetallic random alloys of gold-palladium and ruthenium-palladium supported on titanium dioxide are prepared with a modified metal impregnation method. Gold-palladium/titanium dioxide shows a marked,~27-fold increase in activity (that is, turnover frequency of 0.1?s(-1)) compared with its monometallic counterparts. Although ruthenium-palladium/titanium dioxide is not only exceptionally active (that is, turnover frequency of 0.6?s(-1)), it shows excellent, sustained selectivity to ?-valerolactone (99%). The dilution and isolation of ruthenium by palladium is thought to be responsible for this superior catalytic performance. Alloying, furthermore, greatly improves the stability of both supported nano-alloy catalysts.

| S-EPMC4382690 | biostudies-literature

γ-Valerolactone as Bio-Based Solvent for Nanofiltration Membrane Preparation.

Project description:γ-Valerolactone (GVL) was selected as a renewable green solvent to prepare membranes via the process of phase inversion. Water and ethanol were screened as sustainable non-solvents to prepare membranes for nanofiltration (NF). Scanning electron microscopy was applied to check the membrane morphology, while aqueous rose Bengal (RB) and magnesium sulphate (MgSO4) feed solutions were used to screen performance. Cellulose acetate (CA), polyimide (PI), cellulose triacetate (CTA), polyethersulfone (PES) and polysulfone (PSU) membranes were fine-tuned as materials for preparation of NF-membranes, either by selecting a suitable non-solvent for phase inversion or by increasing the polymer concentration in the casting solution. The best membranes were prepared with CTA in GVL using water as non-solvent: with increasing CTA concentration (10 wt% to 17.5 wt%) in the casting solution, permeance decreased from 15.9 to 5.5 L/m2·h·bar while RB rejection remained higher than 94%. The polymer solubilities in GVL were rationalized using Hansen solubility parameters, while membrane performances and morphologies were linked to viscosity measurements and cloudpoint determination of the casting solutions to better understand the kinetic and thermodynamic aspects of the phase inversion process.

| S-EPMC8228422 | biostudies-literature

Ru@hyperbranched Polymer for Hydrogenation of Levulinic Acid to Gamma-Valerolactone: The Role of the Catalyst Support.

Project description:Hydrogenation of levulinic acid (LA) obtained from cellulose biomass is a promising path for production of γ-valerolactone (GVL)-a component of biofuel. In this work, we developed Ru nanoparticle containing nanocomposites based on hyperbranched pyridylphenylene polymer, serving as multiligand and stabilizing matrix. The functionalization of the nanocomposite with sulfuric acid significantly enhances the activity of the catalyst in the selective hydrogenation of LA to GVL and allows the reaction to proceed under mild reaction conditions (100 °C, 2 MPa of H2) in water and low catalyst loading (0.016 mol.%) with a quantitative yield of GVL and selectivity up to 100%. The catalysts were successfully reused four times without a significant loss of activity. A comprehensive physicochemical characterization of the catalysts allowed us to assess structure-property relationships and to uncover an important role of the polymeric support in the efficient GVL synthesis.

| S-EPMC8776037 | biostudies-literature

Effect of support acidity during selective hydrogenolysis of glycerol over supported palladium-ruthenium catalysts.

Project description:We report the role of the acidity of support during the selectivity hydrogenolysis of glycerol over supported bimetallic palladium-ruthenium (PdRu) catalysts. The PdRu nanoparticles were supported on a series of metal oxides and zeolitic supports via the modified impregnation method and tested for the liquid-phase hydrogenolysis of glycerol using gaseous hydrogen. The relative acid site densities of selected catalysts were determined by ammonia temperature-programmed desorption and pyridine desorption experiments. Based on these studies, we report a direct correlation between the catalytic activity (conversion and 1,2 propane diol yield) and two different acid sites (strong acid sites and very strong acid sites). Besides zeolite-supported catalysts, TiO2 supported PdRu nanoparticles exhibit moderate catalytic activity; however, this catalyst shows high selectivity for the desired C-O bond cleavage to produce C3 products over the undesired C-C bond cleavage to produce < C3 products. This article is part of a discussion meeting issue 'Science to enable the circular economy'.

| S-EPMC7422897 | biostudies-literature

Polymeric Ruthenium Porphyrin-Functionalized Carbon Nanotubes and Graphene for Levulinic Ester Transformations into γ-Valerolactone and Pyrrolidone Derivatives.

Project description:Polymeric ruthenium porphyrin-functionalized carbon nanotubes (Ru-PP/CNTs) were prepared by the metallation of polymeric porphyrin-functionalized carbon nanotubes (PP/CNTs) with Ru3(CO)12, whereas PP/CNTs were obtained by the condensation of terephthaldehyde and pyrrole in the presence of CNTs. The Ru-PP/CNTs have a thin layer of highly cross-linked polymeric ruthenium porphyrin coating over the CNT surface via strong π-π stacking interactions, thus showing a bilayered structure with an amorphous polymeric outer surface and an internal CNT core. Polymeric ruthenium porphyrin-functionalized reduced graphene oxide (Ru-PP/RGO) was prepared with a synthetic procedure similar to Ru-PP/CNTs, with RGO as the internal core. Both Ru-PP/CNTs and Ru-PP/RGO showed excellent catalytic performance toward hydrogenation of biomass-related ethyl levulinate (EL) to γ-valerolactone (GVL) with Ru-centered porphyrin units as the catalytic active species. Under optimized reaction conditions, a GVL yield higher than 99% with a complete conversion of EL was observed over both Ru-PP/CNTs and Ru-PP/RGO. In addition to GVL preparation, the versatile Ru-PP/CNTs can efficiently promote reductive amination of EL with various amines for the synthesis of pyrrolidone derivatives, with the corresponding yields ranging from 96.3 to 88.7%. Moreover, the composite materials of both Ru-PP/CNTs and Ru-PP/RGO behave as heterogeneous catalysts in the reaction system and can be easily reused.

| S-EPMC6641044 | biostudies-literature

Room-Temperature Asymmetric Transfer Hydrogenation of Biomass-Derived Levulinic Acid to Optically Pure γ-Valerolactone Using a Ruthenium Catalyst.

Project description:This study presents a first report on ruthenium-catalyzed asymmetric transfer hydrogenation (ATH) of levulinic acid (LA) to chiral γ-valerolactone (GVL). ATH of LA has been explored with Noyori's chiral catalyst (Ru-TsDPEN) in methanol solvent. Efficacy of ATH reaction of LA was investigated under different reactions conditions such as temperature, catalyst, and hydrogen donor concentration. The effect of various organic tertiary bases along with formic acid (FA) as a hydrogen donor was studied, and N-methylpiperidine with FA (1:1 molar ratio) was revealed as an efficient hydrogen donor for ATH of LA to GVL furnishing chiral GVL with complete conversion and 93% enantiomeric excess (ee). This operationally simple and mild ATH protocol was tested for practical applicability of ATH of LA obtained from biomass waste (rice husk and wheat straw) and furnished chiral GVL with 82% ee.

| S-EPMC6868911 | biostudies-literature

Influence of Sulfuric Acid on the Performance of Ruthenium-based Catalysts in the Liquid-Phase Hydrogenation of Levulinic Acid to ?-Valerolactone.

Project description:The presence of biogenic or process-derived impurities poses a major problem on the efficient catalytic hydrogenation of biomass-derived levulinic acid to ?-valerolactone; hence, studies on their influence on catalyst stability are now required. Herein, the influence of sulfuric acid as feed impurity on the performance of Ru-based heterogeneous catalysts, including Ru/ZrO2 and mono- and bimetallic Ru-on-carbon catalysts in dioxane as solvent, was investigated. The carbon-supported Ru catalysts proved to be very sensitive to minor amounts of sulfuric acid. In stark contrast, Ru/ZrO2 showed a remarkable stability in the presence of the same impurity, which is attributed to the sulfate-ion adsorption capacity of the support. Preferential sulfate adsorption onto the surface of ZrO2 effectively protects the Ru active phase from deactivation by sulfur poisoning. A simple catalyst regeneration strategy was effective in removing adsorbed impurities, allowing efficient catalyst recycling.

| S-EPMC5575478 | biostudies-literature

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