Molekulare Phosphan‐Feststoffkatalysatoren zur Ameisensäurezersetzung in der Bioraffinerie

Hausoul, Peter J. C.; Broicher, Cornelia; Vegliante, Roberta; Göb, Christian R.; Palkovits, Regina

doi:10.1002/ange.201510681

Cited by 12 publications

(4 citation statements)

References 31 publications

(24 reference statements)

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“…It should be noted that in the presence of PPh 3 , chitosan‐Ru could achieve 99 % product yield from the hydrogenation of FF to FAL at 120 °C and transformation of LA or AL to GVL at 160 °C whereas only 80 % yield of GVL was obtained for one pot conversion of FF at 160 °C, which might be attributed to the formation of humins, resulting from the self‐polymerization of furfural at high temperature . Previous studies indicated that PPh 3 can act as an electron‐donor additive and have a weak interaction with Ru 3+ ions, which can facilitate the decomposition of FA, thus being beneficial for the hydrogenation . Therefore, the presence of PPh 3 is also crucially important for the reaction.…”

Section: Resultsmentioning

confidence: 99%

Production of γ‐Valerolactone from One‐Pot Transformation of Biomass‐Derived Carbohydrates Over Chitosan‐Supported Ruthenium Catalyst Combined with Zeolite ZSM‐5

Wang

Zhang

2020

Eur J Org Chem

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It remains as a challenge to directly transform the biomass‐derived C5 carbohydrates, such as furfural (FF) and its upstream product xylose and hemicellulose, to γ‐valerolactone (GVL), a versatile renewable chemical platform, due to various restrictions in the current synthetic strategies. Using formic acid as green hydrogen source, we synthesized the recyclable chitosan‐Ru/PPh3 catalyst system, effective for both the hydrogenation of FF to furfuryl alcohol (FAL) and the reduction of levulinic acid (LA) or ethyl levulinate (EL) to GVL, affording up to 99 % product yields. The combination of chitosan‐Ru/PPh3 with ZSM‐5 could successfully achieve up to 79 % yield of GVL from one‐pot conversion of FF under mild condition. Preliminary studies indicated that this method could also be applied to the direct conversion of biomass‐derived C5 carbohydrates such as xylose and hemicellulose to GVL in 37 % or 30 % yield, respectively.

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Section: Resultsmentioning

confidence: 99%

Production of γ‐Valerolactone from One‐Pot Transformation of Biomass‐Derived Carbohydrates Over Chitosan‐Supported Ruthenium Catalyst Combined with Zeolite ZSM‐5

Wang

Zhang

2020

Eur J Org Chem

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“…No Ru leaching was detected after a turnover number of 71 000, which corresponds to 20 full cycles of full conversion. Palkovits et al . used porous phosphorous‐based phenyl‐polymers as the support in a similar catalytic system.…”

Section: Catalytic Decomposition Of Bio‐based Formic Acid Solutionsmentioning

confidence: 99%

Biogenic Formic Acid as a Green Hydrogen Carrier

Preuster

Albert

2018

Energy Tech

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Formic acid (FA) is an important platform chemical that has numerous applications in the chemical and agricultural industries, as well as in the leather industry. To date, FA is exclusively produced from fossil raw materials using either carbonylation of methanol or acidolysis of formates. Here, sustainable and environmentally friendly approaches to produce biogenic FA from biomass (e.g., OxFA‐process) are presented and combined with different approaches for the catalytic decomposition of bio‐based FA solutions. Several homogeneous and heterogeneous approaches for the catalytic decomposition of aqueous FA to hydrogen and CO2 are compared for their applicability. Moreover, their technical applications in fuel cells, as energy storage vectors, and as hydrogen storage molecules are discussed.

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“…For three‐dimensionally crosslinked polymers a high specific surface area is expected as can be seen for different examples such as hypercrosslinked polymers and polyphosphines, which are also applied in catalytic reactions . However, the herein synthesized amorphous polyamine does not exhibit a permanent porosity in dry state although it is three‐dimensionally crosslinked.…”

Section: Resultsmentioning

confidence: 74%

Solid Molecular Frustrated Lewis Pairs in a Polyamine Organic Framework for the Catalytic Metal‐free Hydrogenation of Alkenes

et al. 2018

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We report for the first time a metal‐free heterogeneously catalyzed hydrogenation using a semi‐solid frustrated Lewis pair (FLP). The catalyst consists of a solid polyamine organic framework and molecular tris(pentafluorophenyl)borane (BCF) that form a semi‐immobilized FLP in situ in the catalytic hydrogenation of diethyl benzylidenemalonate. 11B NMR spectroscopy proves the successful hydrogen activation by the FLP. Furthermore, the B−N interactions between the polyamine and BCF are investigated by IR and solid state NMR spectroscopy. The FLP 1,4‐diazabicyclo[2.2.2]octane (DABCO)/BCF, which combines the features of a FLP and a classical Lewis adduct, functions as molecular reference in both, catalysis and characterization. Furthermore, computational studies enable a better insight into the hydrogen activation through DABCO/BCF and polyamine/BCF.

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Molekulare Phosphan‐Feststoffkatalysatoren zur Ameisensäurezersetzung in der Bioraffinerie

Cited by 12 publications

References 31 publications

Production of γ‐Valerolactone from One‐Pot Transformation of Biomass‐Derived Carbohydrates Over Chitosan‐Supported Ruthenium Catalyst Combined with Zeolite ZSM‐5

Production of γ‐Valerolactone from One‐Pot Transformation of Biomass‐Derived Carbohydrates Over Chitosan‐Supported Ruthenium Catalyst Combined with Zeolite ZSM‐5

Biogenic Formic Acid as a Green Hydrogen Carrier

Solid Molecular Frustrated Lewis Pairs in a Polyamine Organic Framework for the Catalytic Metal‐free Hydrogenation of Alkenes

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