Abstract:The synthesis of 2,5-dimethylfuran (DMF) from 5-hydroxymethylfurfural (HMF) is a highly attractive route to a renewable fuel. However, achieving high yields in this reaction is a substantial challenge. Here it is described how PtCo bimetallic nanoparticles with diameters of 3.6 ± 0.7 nm can solve this problem. Over PtCo catalysts the conversion of HMF was 100% within 10 min and the yield to DMF reached 98% after 2 h, which substantially exceeds the best results reported in the literature. Moreover, the synthet… Show more
“…32,33 Recently, the outstanding hydrogenolysis of HMF to DMF with a 98% yield at 180°C for 2 h (10 bar H 2 gas) was reported, in which bimetallic nanoparticles in hollow carbon nanospheres were used to avoid the aggregation of the nanometal catalyst. 31 However, to the best our knowledge, our direct conversion from fructose to DMF is demonstrated for the first time with impressive performance under milder conditions, which is partly attributed to the efficient heat and mass transfer in the tube-in-tube microreactor. The overall conversion and yield of DMF directly from fructose by the integrated microfluidic transformation platform requires only simple operation and does not require any separation or removal steps of impurities from products.…”
Section: Ternary Phase Conversion To Furan Chemicals From Fructosementioning
confidence: 90%
“…The Pt metal catalyst nearly completed the conversion of HMF (98%) with a low yield of DMF (20%) due to the overhydrogenated product (1b, 53% yield), as expected. 31 In the bimetallic catalysts, the catalytic activity was generally higher than those of the monometallic catalysts. In particular, the Ru/Cu catalyst exhibited the best activity with a 78% yield of DMF, assuring that the Ru/Cu/Fe 3 O 4 / N-rGO catalyst was suitable for the microfluidic hydrogenolysis reaction in the ternary phase.…”
Section: Ternary Phase Conversion To Furan Chemicals From Fructosementioning
The sustainable green chemistry associated with lignocellulosic biomass is of current interest for producing various chemical feedstocks via multi-step transformation processes. Here we introduce a chemical platform system for the multicomponent cascade transformation of natural lignocellulosic biomass resources. We demonstrate the concept by developing an integrated continuous two-step microfluidic system as a tandem transformation platform for direct conversion of fructose to diverse furan chemicals with excellent yields up to 99% via decarbonylation, etherification, oxidation and hydrogenolysis of a 5-hydroxymethylfurfural (HMF) intermediate. A sequential two-step process is utilized to complete the dehydration of fructose in the surface acid catalyst at 150°C for 6 min, which is followed by the four types of HMF conversion in a binary or ternary phase to produce furfuryl alcohol (94% yield), 5-ethoxymethylfurfural (99%), 2,5-diformylfuran (82%) and 2,5-dimethylfuran (90%) with magnetic-based heterogeneous catalysts at 70-150°C for 6-60 min. This innovative tandem microfluidic platform enables precise control of the reaction temperature and time for each individual biomass conversion step in a one-flow manner with no separation and purification steps for intermediates and catalysts.
“…32,33 Recently, the outstanding hydrogenolysis of HMF to DMF with a 98% yield at 180°C for 2 h (10 bar H 2 gas) was reported, in which bimetallic nanoparticles in hollow carbon nanospheres were used to avoid the aggregation of the nanometal catalyst. 31 However, to the best our knowledge, our direct conversion from fructose to DMF is demonstrated for the first time with impressive performance under milder conditions, which is partly attributed to the efficient heat and mass transfer in the tube-in-tube microreactor. The overall conversion and yield of DMF directly from fructose by the integrated microfluidic transformation platform requires only simple operation and does not require any separation or removal steps of impurities from products.…”
Section: Ternary Phase Conversion To Furan Chemicals From Fructosementioning
confidence: 90%
“…The Pt metal catalyst nearly completed the conversion of HMF (98%) with a low yield of DMF (20%) due to the overhydrogenated product (1b, 53% yield), as expected. 31 In the bimetallic catalysts, the catalytic activity was generally higher than those of the monometallic catalysts. In particular, the Ru/Cu catalyst exhibited the best activity with a 78% yield of DMF, assuring that the Ru/Cu/Fe 3 O 4 / N-rGO catalyst was suitable for the microfluidic hydrogenolysis reaction in the ternary phase.…”
Section: Ternary Phase Conversion To Furan Chemicals From Fructosementioning
The sustainable green chemistry associated with lignocellulosic biomass is of current interest for producing various chemical feedstocks via multi-step transformation processes. Here we introduce a chemical platform system for the multicomponent cascade transformation of natural lignocellulosic biomass resources. We demonstrate the concept by developing an integrated continuous two-step microfluidic system as a tandem transformation platform for direct conversion of fructose to diverse furan chemicals with excellent yields up to 99% via decarbonylation, etherification, oxidation and hydrogenolysis of a 5-hydroxymethylfurfural (HMF) intermediate. A sequential two-step process is utilized to complete the dehydration of fructose in the surface acid catalyst at 150°C for 6 min, which is followed by the four types of HMF conversion in a binary or ternary phase to produce furfuryl alcohol (94% yield), 5-ethoxymethylfurfural (99%), 2,5-diformylfuran (82%) and 2,5-dimethylfuran (90%) with magnetic-based heterogeneous catalysts at 70-150°C for 6-60 min. This innovative tandem microfluidic platform enables precise control of the reaction temperature and time for each individual biomass conversion step in a one-flow manner with no separation and purification steps for intermediates and catalysts.
“…Figure 3 contains an example of such a STEM-EELS analysis that has been performed on a sample which was having a porous carbon (C) material functionalized with oxidized bimetallic FeCo-NPs. Such materials are promising candidates for the energy related applications [14]. It can be seen from Figure 3a that the oxidized FeCo-NPs were uniformly embedded in porous C material and while the corresponding EELS spectrum not only revealed the presence of all the expected elements in the sample but it also allowed the analysis of Fe-L23 and Co-L23 white lines to determine the oxidation states of both Fe and Co elements [13].…”
Section: Analytical Electron Microscopy Of Nano-materialsmentioning
Abstract. The field of nanotechnology is about research and development on materials whose at least one dimension is in the range of 1 to 100 nanometers. In recent years, the research activity for developing nano-materials has grown exponentially owing to the fact that they offer better solutions to the challenges faced by various fields such as energy, food, and environment. In this paper, the importance of transmission electron microscopy (TEM) based techniques is demonstrated for investigating the properties of nano-materials. Specifically the nano-materials that are investigated in this report include gold nano-particles (Au-NPs), silver atom-clusters (Ag-ACs), tantalum single-atoms (Ta-SAs), carbon materials functionalized with iron cobalt (Fe-Co) NPs and titania (TiO 2 ) NPs, and platinum loaded Ceria (Pt-CeO 2 ) Nano composite. TEM techniques that are employed to investigate nano-materials include aberration corrected bright-field TEM (BF-TEM), high-angle dark-field scanning TEM (HAADF-STEM), electron energy-loss spectroscopy (EELS), and BF-TEM electron tomography (ET). With the help presented of results in this report, it is proved herein that as many TEM techniques as available in a given instrument are essential for a comprehensive nano-scale analysis of nanomaterials.
“…For example, Schüth and co-workers tested a method involving thermal reduction of metal ions confined in carbon nanopores to obtain noble-metal nanoparticles encapsulated in hollow carbon nanospheres. [23][24][25] However, no matter how the as-synthesized metal nanocrystals were prepared, by surfactant-assisted, microemulsion or polyol reaction methods, [26][27][28] the ligands stabilizing the as-synthesized metal nanocrystals weakened the interactions between metal active sites and reactants, resulting in a decreased catalytic activity. Furthermore, because of the lack of suitable functional groups in the inert pre-synthesized carbon spheres, the post-synthetically loaded metal nanoparticles were non-uniform and randomly distributed onto the carbon spheres.…”
N-doped mesoporous carbon nanospheres (N-MCN@M) impregnated with uniformly dispersed noble-metal (Au, Pt, Rh, Ru, Ag, Pd and Ir) nanoparticles are rationally designed and synthesized for hydrogenation reactions. This facile and generally applicable synthetic strategy ensured confinement of the noble-metal nanoparticles within different carbon morphologies, including mesoporous spheres, hollow particles and core-shell particles. High loading of the noble-metal nanoparticles from 8 to 44% was accomplished by tuning the initial concentration of metal salts. Even at very high loadings (440 wt%), a homogeneous dispersion of uniform metal nanoparticles throughout the carbon nanostructures was achieved. The proposed synthesis is also well suited for the fabrication of carbon spheres loaded with bimetallic nanoparticles (AuPt, AuRh and PtRh). Examination of these metal-loaded carbon particles as catalysts for the hydrogenation of benzaldehyde gave 100% selectivity toward carbonyl group at room and higher reaction temperatures. The outstanding performance of Au nanoparticles gave an unprecedented turn over frequency 2-4 times greater than those of Pt nanoparticles with the same size, loading and support.
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