Cascade catalytic hydrogenation–cyclization of methyl levulinate to form γ-valerolactone over Ru nanoparticles supported on a sulfonic acid-functionalized UiO-66 catalyst

Lin, Zhenzhen; Cai, Xiaoxiong; Fu, Yanghe; Zhu, Weidong; Zhang, Fu‐Min

doi:10.1039/c7ra06293a

Cited by 45 publications

(32 citation statements)

References 48 publications

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“…A one-pot catalytic hydrogenation strategy for converting methyl levulinate into g-valerolactone was developed using a bifunctional catalyst composed of metallic Ru NPs deposited on a SO 3 H-functionalised UiO-66. 254 The resulting catalyst showed a 81% yield of g-valerolactone under mild reaction conditions, which was maintained even after five recycles of the catalyst (entry 12, Table 2). The catalytic performance of Ru/SO 3 H-UiO-66 was attributed to synergistic effect of imbedded tiny metallic Ru NPs (2-4 nm diameter) and abundant Brønsted acidic sites of SO 3 H-UiO-66 support, hereby outperforming a Ru/C catalyst.…”

Section: Bifunctionalised Mofsmentioning

confidence: 97%

Functionalised heterogeneous catalysts for sustainable biomass valorisation

et al. 2018

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Efficient transformation of biomass to value-added chemicals and high-energy density fuels is pivotal for a more sustainable economy and carbon-neutral society. In this framework, developing potential cascade chemical processes using functionalised heterogeneous catalysts is essential because of their versatile roles towards viable biomass valorisation. Advances in materials science and catalysis have provided several innovative strategies for the design of new appealing catalytic materials with well-defined structures and special characteristics. Promising catalytic materials that have paved the way for exciting scientific breakthroughs in biomass upgrading are carbon materials, metal-organic frameworks, solid phase ionic liquids, and magnetic iron oxides. These fascinating catalysts offer unique possibilities to accommodate adequate amounts of acid-base and redox functional species, hence enabling various biomass conversion reactions in a one-pot way. This review therefore aims to provide a comprehensive account of the most significant advances in the development of functionalised heterogeneous catalysts for efficient biomass upgrading. In addition, this review highlights important progress ensued in tailoring the immobilisation of desirable functional groups on particular sites of the above-listed materials, while critically discussing the role of consequent properties on cascade reactions as well as on other vital processes within the bio-refinery. Current challenges and future opportunities towards a rational design of novel functionalised heterogeneous catalysts for sustainable biomass valorisation are also emphasized.

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Section: Bifunctionalised Mofsmentioning

confidence: 97%

Functionalised heterogeneous catalysts for sustainable biomass valorisation

et al. 2018

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“…[109] Acid-base titrations indicated that the acidity of Ru/UiO-66-SO 3 H was 0.35 mmol g À 1 . A dual functional catalyst, namely, Ru NPs deposited by wet impregnation method on sulfonic acid-functionalized UiO-66 (Ru/UiO-66-SO 3 H) was prepared and its activity was evaluated in the conversion of methyl levulinate into GVL (Scheme 19).…”

Section: Other Metal Npsmentioning

confidence: 99%

“…A dual functional catalyst, namely, Ru NPs deposited by wet impregnation method on sulfonic acid-functionalized UiO-66 (Ru/UiO-66-SO 3 H) was prepared and its activity was evaluated in the conversion of methyl levulinate into GVL (Scheme 19). [109] Acid-base titrations indicated that the acidity of Ru/UiO-66-SO 3 H was 0.35 mmol g À 1 . TEM images confirmed the uniform distribution of Ru NPs on UiO-66-SO 3 H matrix with the size ranging between 2-4 nm.…”

Section: Other Metal Npsmentioning

confidence: 99%

Engineering UiO‐66 Metal Organic Framework for Heterogeneous Catalysis

et al. 2019

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frameworks (MOFs) are currently attracting considerable attention as heterogeneous catalysts at moderate temperatures, mainly for liquid-phase reactions. Since structural stability is one of the major concerns for the use of MOFs in catalysis, particularly considering that frequently some of the reported MOF materials are very unstable, the interest in this area has been focused on those MOFs exhibiting the highest structural robustness, UiO-66 being among the most widely used. Two introductory sections deal with the synthesis, structure and main properties of UiO-66, including its remarkable thermal (up to 350°C) and chemical (aqueous solution in a wide pH range) stability. The main body of the review summarizes those examples of using UiO-66 in catalysis grouped according to the nature of the active sites, starting with the use of UiO-66 as Lewis acids. In this section, emphasis has been made in the recent strategies to create structural defects in a controlled way that generate Lewis acidity. Other sections cover examples illustrating substituted terephthalate as active sites and the evidence that there is a synergy between acid and basic sites in close proximity that make some of these UiO-66 with substituents at the linker to act as dual acid-base catalysts. Other sections are focused on the use of UiO-66 as hosts of metal nanoparticles, metal oxides and other host, remarking the influence that the nature of UiO-66 and the possible presence of substituents in the framework play on the activity of the incorporated guest. The last section summarizes the current state of the art in the use of UiO-66 in catalysis and provides our views on future developments regarding the application of UiO-66 in industrial processes.

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“…A bifunctional catalyst Ru/@SO 3 H-UiO-66(Zr) was prepared by depositing Ru nanoparticles on a sulfonic acid-functionalized Zr-based metal-organic framework (SO 3 H-UiO-66) [131]. Its efficiency has been proven in a high-yield one-pot upgrade strategy for converting biomass-derived methyl levulinate (ML) into γ-valerolactone (GVL) by obtaining a quantitative (100%) yield of GVL (80 • C, 0.5 MPa H 2 , 4 h, aqueous media).…”

Section: Hybrid Materials In the Form Of Mof Host Matrices Containingmentioning

confidence: 99%

Metal–Organic Frameworks-Based Catalysts for Biomass Processing

2018

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: Currently, metal–organic frame works (MOFs) as novel hybrid nanoporous materials are a top research interest, including endeavors in heterogeneous catalysis. MOF materials are promising heterogeneous catalytic systems due to their unique characteristics, such as a highly ordered structure, a record high surface area and a compositional diversity, which can be precisely tailored. Very recently, these metal-organic matrices have been proven as promising catalysts for biomass conversion into value-added products. The relevant publications show that the structure of MOFs can contribute essentially to the advanced catalytic performance in processes of biomass refining. This review aims at the consideration of the different ways for the rational design of MOF catalysts for biomass processing. The particular characteristics and peculiarities of the behavior of different MOF based catalytic systems including hybrid nanomaterials and composites will be also discussed by illustrating their outstanding performance with appropriate examples relevant to biomass catalytic processing.

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Cascade catalytic hydrogenation–cyclization of methyl levulinate to form γ-valerolactone over Ru nanoparticles supported on a sulfonic acid-functionalized UiO-66 catalyst

Abstract: The developed Ru/SO3H-UiO-66 exhibits a novel synergistic catalysis to upgrade methyl levulinate into γ-valerolactone under mild conditions in water.

Cited by 45 publications

References 48 publications

Functionalised heterogeneous catalysts for sustainable biomass valorisation

Functionalised heterogeneous catalysts for sustainable biomass valorisation

Engineering UiO‐66 Metal Organic Framework for Heterogeneous Catalysis

Metal–Organic Frameworks-Based Catalysts for Biomass Processing

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