Hydrogenation of levulinic acid to γ-valerolactone over Pd@UiO-66-NH2 with high metal dispersion and excellent reusability

Feng, Jian; Li, Min; Zhong, Yanhui; Xu, Yuliang; Meng, Xianglong; Zhao, Zhiwei; Feng, Chang

doi:10.1016/j.micromeso.2019.109858

Cited by 45 publications

(33 citation statements)

References 47 publications

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“…Similar results were also observed for the Pd/UiO-66- 7 material. The Pd/UiO-66-NO 2 - 7 (IMP) exhibits a lower specific surface area ( S BET = 519 m 2 ·g −1 ) and a smaller pore volume compared to Pd/UiO-66-NO 2 - 7 , due to the partial blockage by Pd particles at the pore mouths of UiO-66-NO 2 - 7 [ 31 ]. The dispersion of Pd was determined by CO pulse chemisorption, and the results are listed in Table 1 .…”

Section: Resultsmentioning

confidence: 99%

“…The thermal treatment will result in the formation of defects in the MOF structure and will enhance the specific surface area, pore size, and Lewis acid sites [ 29 , 30 ]. The tunable features of MOFs ensure the encapsulation and confinement of metal nanoparticles by forming a weak bond between the metal precursor and unsaturated metal center, thus improving the metal dispersion and preventing metal leaching [ 31 ].…”

Section: Introductionmentioning

confidence: 99%

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Hydrogenative Ring-Rearrangement of Furfural to Cyclopentanone over Pd/UiO-66-NO2 with Tunable Missing-Linker Defects

Wang

Yang

et al. 2021

Molecules

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Upgrading furfural (FAL) to cyclopentanone (CPO) is of great importance for the synthesis of high-value chemicals and biomass utilization. The hydrogenative ring-rearrangement of FAL is catalyzed by metal-acid bifunctional catalysts. The Lewis acidity is a key factor in promoting the rearrangement of furan rings and achieving a high selectivity to CPO. In this work, highly dispersed Pd nanoparticles were successfully encapsulated into the cavities of a Zr based MOF, UiO-66-NO2, by impregnation using a double-solvent method (DSM) followed by H2 reduction. The obtained Pd/UiO-66-NO2 catalyst showed a significantly better catalytic performance in the aforementioned reaction than the Pd/UiO-66 catalyst due to the higher Lewis acidity of the support. Moreover, by using a thermal treatment. The Lewis acidity can be further increased through the creating of missing-linker defects. The resulting defective Pd/UiO-66-NO2 exhibited the highest CPO selectivity and FAL conversion of 96.6% and 98.9%, respectively. In addition, the catalyst was able to maintain a high activity and stability after four consecutive runs. The current study not only provides an efficient catalytic reaction system for the hydrogenative ring-rearrangement of furfural to cyclopentanone but also emphasizes the importance of defect sites.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Hydrogenative Ring-Rearrangement of Furfural to Cyclopentanone over Pd/UiO-66-NO2 with Tunable Missing-Linker Defects

Wang

Yang

et al. 2021

Molecules

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“…Noble metal catalysts (Au, Ru, Pt, Ir, Pd, Rh, Os, Ag) are commonly used catalysts in the preparation of GVL. Recently, Feng et al [34] used UiO-66À NH 2 as a support to encapsulate dispersed Pd particles (Figure 2a). The developed Pd@UiO-66À NH 2 catalyst was active, selective and durable for the hydrogenation of LA to GVL at a relatively lower temperature (140°C) and in the presence of molecular hydrogen.…”

Section: Noble Metal Catalystsmentioning

confidence: 99%

“…a) Schematic illustration of Pd@UiO-66À NH 2 catalyst for LA hydrogenating to GVL (reprinted with permission from Ref [34]…”

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confidence: 99%

Falling Leaves Return to Their Roots: A Review on the Preparation of γ‐Valerolactone from Lignocellulose and Its Application in the Conversion of Lignocellulose

Liu

et al. 2020

ChemSusChem

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γ‐Valerolactone (GVL), derived from renewable lignocellulosic biomass, has been considered as a cost‐competitive and green platform chemical. With the increasingly prominent environmental problems, a deep understanding of the preparation and transformation of GVL is highly needed. Based on the latest progress made with GVL, preparation and applications of GVL are summarized and discussed in this Review. In particular, the state‐of‐the‐art in catalytic production of GVL is described based on the use of noble‐metal and non‐noble‐metal catalysts. The application of GVL for the valorization of lignocellulose would improve the yield of target products such as sugar monomers and furfural. Thus, GVL can be produced from lignocellulose and simultaneously it can also be used for the valorization of lignocellulose, just as in the sustainable and renewable cycle, “the falling leaves returns to their roots”. This Review is expected to provide valuable reference and new proposal for the further development and better utilization of GVL.

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“…Keeping these requirements in mind, metal-organic frameworks (MOFs) are novel porous materials based on inorganic metals and multidentate organic ligands, which can not only act as catalytic materials themselves but also serve as support for diverse catalytic units (e.g., metal and metal oxide nanoparticles, organic functional groups). The unique structural features of MOFs promote the metal dispersion and avoid metal leaching, and they can be easily modified with additional functionalities, thereby leading to outstanding catalytic performance in a myriad of different chemical transformations [9][10][11], including, for example, the production of GVL [12][13][14]. In this regard, our group has reported the use of a zirconium-based MOF, UiO-66, to carry out the transformation of methyl levulinate (ML) to GVL via catalytic transfer hydrogenation (CTH) under continuous flow [12].…”

Section: Introductionmentioning

confidence: 99%

Mechanochemical Synthesis of Nickel-Modified Metal–Organic Frameworks for Reduction Reactions

et al. 2021

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In this work, we report the incorporation of nickel oxide nanoparticles into a metal–organic framework (MOF) structure by a solvent-free mechanochemical strategy. In particular, the zirconium-based MOF UiO-66 was modified with different Ni loadings and characterized using complementary techniques including X-ray diffraction (XRD), N2 porosimetry and X-ray photoelectron spectroscopy (XPS). The catalytic potential of the as-prepared Ni/UiO-66 materials in the hydrogenation reaction of methyl levulinate using 2-propanol as hydrogen donor solvent has been investigated under flow conditions. Under optimized conditions, the 5%Ni/UiO-66 led to the best catalytic performance (70% yield, 100% selectivity to gamma-valerolactone), which could be attributed to the higher content of the Ni species within the MOF structure. The obtained results are promising and contribute to highlighting the great potential of MOFs in biomass upgrading processes, opening the path to the sustainable development of the chemical industry.

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Hydrogenation of levulinic acid to γ-valerolactone over Pd@UiO-66-NH2 with high metal dispersion and excellent reusability

Cited by 45 publications

References 47 publications

Hydrogenative Ring-Rearrangement of Furfural to Cyclopentanone over Pd/UiO-66-NO2 with Tunable Missing-Linker Defects

Hydrogenative Ring-Rearrangement of Furfural to Cyclopentanone over Pd/UiO-66-NO2 with Tunable Missing-Linker Defects

Falling Leaves Return to Their Roots: A Review on the Preparation of γ‐Valerolactone from Lignocellulose and Its Application in the Conversion of Lignocellulose

Mechanochemical Synthesis of Nickel-Modified Metal–Organic Frameworks for Reduction Reactions

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