Conversion of Levulinic Acid to γ-Valerolactone over Few-Layer Graphene-Supported Ruthenium Catalysts

Xiao, Chaoxian; Goh, Tian Wei; Qi, Zhiyuan; Goes, Shannon; Brashler, Kyle; Perez, Christopher; Huang, Wenyu

doi:10.1021/acscatal.5b02673

Cited by 148 publications

(92 citation statements)

References 52 publications

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“…The ability of Ru/FLG (2 wt. %) to catalyze LA hydrogenation to GVL was recently demonstrated [22]. In this study, quantitative LA conversion with 100% GVL selectivity was obtained in water at room temperature (40 bar H 2 , 12 h).…”

Section: Introductionmentioning

confidence: 70%

“…For Ru/C, slow though irreversible deactivation was observed in water, due to Ru sintering and a reduction in the BET surface area due to coke deposition [17][18][19]. Other forms of carbon, like carbon nanotubes and few-layer graphene (FLG), have also been identified as promising support materials for many metal catalysts [20][21][22]. Advantages of CNTs as a support compared to active carbons are a higher catalyst stability and lower intra-particle diffusion limitations of reactants [23].…”

Section: Introductionmentioning

confidence: 99%

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Support Screening Studies on the Hydrogenation of Levulinic Acid to γ-Valerolactone in Water Using Ru Catalysts

et al. 2016

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γ-Valerolactone (GVL) has been identified as a sustainable platform chemical for the production of carbon-based chemicals. Here we report a screening study on the hydrogenation of levulinic acid (LA) to GVL in water using a wide range of ruthenium supported catalysts in a batch set-up (1 wt. % Ru, 90 • C, 45 bar of H 2 , 2 wt. % catalyst on LA). Eight monometallic catalysts were tested on carbon based(C, carbon nanotubes (CNT)) and inorganic supports (Al 2 O 3 , SiO 2 , TiO 2 , ZrO 2 , Nb 2 O 5 and Beta-12.5). The best result was found for Ru/Beta-12.5 with almost quantitative LA conversion (94%) and 66% of GVL yield after 2 h reaction. The remaining product was 4-hydroxypentanoic acid (4-HPA). Catalytic activity for a bimetallic RuPd/TiO 2 catalyst was by far lower than for the monometallic Ru catalyst (9% conversion after 2 h). The effects of relevant catalyst properties (average Ru nanoparticle size, Brunauer-Emmett-Teller (BET) surface area, micropore area and total acidity) on catalyst activity were assessed.

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Section: Introductionmentioning

confidence: 70%

Section: Introductionmentioning

confidence: 99%

Support Screening Studies on the Hydrogenation of Levulinic Acid to γ-Valerolactone in Water Using Ru Catalysts

et al. 2016

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“…This is because the hydrogenation of keto group is catalysed by a combined effort of both the ruthenium active site and the support. The support activates carbonyl group of LA, while ruthenium efficiently dissociates H 2 [31,33,34]. Ruthenium is an excellent hydrogenation catalyst, and ZrO 2 is a known support for hydrogenation, [40][41][42] dehydration, [43] esterification [38], and isomerization reactions [44][45][46][47].…”

Section: Resultsmentioning

confidence: 99%

“…The problem is that small changes in any number of parameters often cause large variance in catalyst performance. Using different supports and even using different phases of the same compound [30][31][32] alters conversion and yield [17]. Another parameter that influences catalyst performance is the metal dispersion on the surface.…”

Section: Introductionmentioning

confidence: 99%

“…Another parameter that influences catalyst performance is the metal dispersion on the surface. In general, smaller Ru particles are more active, but the catalyst is less robust [17,19,31,33]. Also, it is reported in literature that mixing acid catalysts with Ru metal catalysts promoted hydrogenation and bifunctional catalysts are active and recyclable in aqueous solution [18,34].…”

Section: Introductionmentioning

confidence: 99%

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Highly Selective Hydrogenation of Levulinic Acid to γ-Valerolactone Over Ru/ZrO2 Catalysts

et al. 2017

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We studied the catalytic hydrogenation of levulinic acid over zirconia supported ruthenium catalysts. Four different Ru/ZrO 2 catalysts were prepared by different pre-treatments and using different zirconium supports (ZrO x (OH) 4−2x and ZrO 2 ). Although the final compositions of the catalysts are the same, the pre-treatments strongly affect catalytic activity. Remarkably, one of the catalysts gave >99% yield of γ-valerolactone under mild conditions. This catalyst was also robust, and could be recycled at least four times without any loss in activity or selectivity. The activity is attributed to the presence of small ruthenium particles together with acidic sites on the catalyst.Graphical Abstract Pre-treatment changes the performance for ruthenium nanoparticles on zirconia supports, giving TONs over 3500 in the hydrogenation of levulinic acid to γ-valerolactone with over 99% yield. Electronic supplementary materialThe online version of this article

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Carbon‐Support‐Based Heterogeneous Nanocatalysts: Synthesis and Applications in Organic Reactions

2019

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Carbon-based-materials, owing to their wide availability and low cost, have been utilized for a variety of applications including heterogeneous catalysis. Various carbonaceous materials have been used as supports for transition metals or other materials. These support materials have shown their potential for development of green and sustainable approaches to heterogeneous catalysis. In this review, we discuss the utilization of carbon-based materials as supports for heterogeneous catalysts, especially in organic transformations. We have focused our discussions predominantly on four categories of carbonaceous supports, namely graphene (including, graphene oxide (GO) and reduced graphene oxide (RGO)), graphitic carbon nitride (GCN), carbon nanotubes (CNT) and activated carbon (AC) for various organic transformation reactions. Several approaches for the synthesis of these materials along with their application as heterogeneous catalysts for organic transformation reactions have been elaborated in detail. In addition, different aspects of organic synthesis, including hydrogenation, oxidation, reduction, condensation, and multi-component reactions, catalyzed by these materials have been discussed. Furthermore, organic transformations leading to the sustainable synthesis of valuable products from biomass have also been discussed. Finally, after a brief summary, the future perspectives of this very interesting class of materials are provided. Figure 1. Different types of carbon-support-based materials used as heterogeneous catalysts for organic transformations.

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Conversion of Levulinic Acid to γ-Valerolactone over Few-Layer Graphene-Supported Ruthenium Catalysts

Cited by 148 publications

References 52 publications

Support Screening Studies on the Hydrogenation of Levulinic Acid to γ-Valerolactone in Water Using Ru Catalysts

Support Screening Studies on the Hydrogenation of Levulinic Acid to γ-Valerolactone in Water Using Ru Catalysts

Highly Selective Hydrogenation of Levulinic Acid to γ-Valerolactone Over Ru/ZrO2 Catalysts

Carbon‐Support‐Based Heterogeneous Nanocatalysts: Synthesis and Applications in Organic Reactions

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