Dataset Information

Renewable Cyclopentanol From Catalytic Hydrogenation-Rearrangement of Biomass Furfural Over Ruthenium-Molybdenum Bimetallic Catalysts.

ABSTRACT: Biomass furfural-like compounds are chemicals that cannot be extracted from fossil materials, through which a large number of fine chemicals and fuel additives can be opened up, but one big efficiency problem during the transformation is the accumulation of oligomers. Here, we propose a novel and efficient Ru-Mo bimetallic catalyst for selective hydrogenation-rearrangement of furfural-like compounds. The result showed that an unprecedented rearrangement product selectivity of 89.1% to cyclopentanol was achieved under an optimized reaction condition over a 1%Ru-2.5%Mo/CNT catalyst reduced at 600°C. Subsequent characterization suggested that the catalyst presented with weak acidity and strong hydrogenation activity for the reaction, which not only ensures the smooth hydrogenation-rearrangement reaction but also inhibits the accumulation of furan polymers. These findings provide a convenient strategy to tune the catalytic performance of Mo-based catalysts by controlling the reduction and carburization conditions, which appear to be versatile for the rearrangement of furans and similar compounds.

SUBMITTER: Meng S

PROVIDER: S-EPMC7775491 | biostudies-literature | 2020

REPOSITORIES: biostudies-literature

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Renewable Cyclopentanol From Catalytic Hydrogenation-Rearrangement of Biomass Furfural Over Ruthenium-Molybdenum Bimetallic Catalysts.

Meng Shihang S Weng Yujing Y Wang Xiaolong X Yin Hongxing H Wang Zhenfei Z Sun Qi Q Fan Maohong M Zhang Yulong Y

Frontiers in bioengineering and biotechnology 20201218

Biomass furfural-like compounds are chemicals that cannot be extracted from fossil materials, through which a large number of fine chemicals and fuel additives can be opened up, but one big efficiency problem during the transformation is the accumulation of oligomers. Here, we propose a novel and efficient Ru-Mo bimetallic catalyst for selective hydrogenation-rearrangement of furfural-like compounds. The result showed that an unprecedented rearrangement product selectivity of 89.1% to cyclopenta ...[more]

PMID: 33392177

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Project description:Bimetallic heterogeneous catalysts combining group 9 metals (Rh, Ir) or group 10 metals (Ni, Pd, Pt) with Mo on a silica-based support have been synthesized via surface organometallic chemistry and assessed in their catalytic activity for the hydrodeoxygenation (HDO) of alcohols with particular emphasis on the structural evolution of the catalysts and the role of Mo. The investigation was conducted with an air-free approach to isolate any sample alterations exclusively to those caused by the reaction. Structural analysis was performed using a combination of (S)TEM, IR, and XAS. It was found that Ir-Mo/SiO2, Rh-Mo/SiO2, and Pt-Mo/SiO2 display high activity for primary, secondary, and tertiary alcohol deoxygenation, while Pd-Mo/SiO2 selectively catalyses tertiary alcohol deoxygenation. Other combinations as well as the corresponding monometallic materials do not display the same activity. X-ray absorption spectroscopy confirmed metallic states for M (M = Ni, Rh, Pd, Ir, or Pt), while Mo K-edge XANES showed varying amounts of Mo(0), Mo(iv) and Mo(vi) depending on the metal counterpart in fresh materials, and indicated complete conversion of Mo(vi) to lower oxidation states (IV and 0) during the reaction. For Rh, Pd, Ir, and Pt, alloy formation (M-Mo) was identified via M-Mo paths in EXAFS and supported by CO-IR spectroscopy. In contrast to Ir, Rh, and Pt, where some Mo(0) is present at the nanoparticle surface, Pd-Mo forms an alloy but likely retains Mo in the nanoparticle core, as suggested by CO-IR spectroscopy and CO-chemisorption. Reactivity studies suggest that tertiary alcohols primarily undergo dehydration-hydrogenation, evidenced by olefin formation with MoO x /SiO2, as well as Ir/SiO2 and Ir-Mo/SiO2 under inert conditions. In contrast, primary and secondary alcohols follow a different mechanism, correlated with the presence of metallic Mo species on the nanoparticle surface, highlighting their role in C-O bond activation. These findings provide new insights into the structure-activity relationships of Mo-based bimetallic catalysts, underscoring the influence of Mo in different oxidation states and strong substrate dependence on mechanistic pathways.

Dataset Information

Renewable Cyclopentanol From Catalytic Hydrogenation-Rearrangement of Biomass Furfural Over Ruthenium-Molybdenum Bimetallic Catalysts.

Publications

Renewable Cyclopentanol From Catalytic Hydrogenation-Rearrangement of Biomass Furfural Over Ruthenium-Molybdenum Bimetallic Catalysts.

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