Bioethanol Production from Unpretreated Cellulose under Neutral Selfsustainable Hydrolysis/Hydrogenolysis Conditions Promoted by the Heterogeneous Pd/Fe3O4 Catalyst.
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ABSTRACT:
SUBMITTER: Gumina B
PROVIDER: S-EPMC6648557 | BioStudies | 2019-01-01
REPOSITORIES: biostudies
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Project description:In this work, Cu nanoparticles (Cu NPs, 2-20 nm) supported on Hydrotalcite catalysts exhibit enhanced selectivity for ?-valerolactone (GVL) during hydrogenolysis of levulinic acid (LA). At 260 °C, over 3 wt% Cu achieved 87.5% of LA conversion with a maximum GVL selectivity (95%). In contrast, LA hydrogenolysis over 3Cu/Hydrotalcite catalyst is highly active and stable toward the production of GVL due to balanced acido-basicity and higher Cu dispersion with ultrasmall particle sizes, which are investigated through the temperature programmed desorption (TPD) of ammonia, N2O titration, and transmission electron microscopy (TEM) analysis. Hydrotalcite in combination with inexpensive Cu catalyst is found to be an efficient and environmentally benign for LA hydrogenolysis.
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Project description:Monometallic cerium layered double hydroxides (Ce-LDH) supports were successfully synthesized by a homogeneous alkalization route driven by hexamethylenetetramine (HMT). The formation of the Ce-LDH was confirmed and its structural and compositional properties studied by XRD, SEM, XPS, iodometric analyses and TGA. HT-XRD, N2-sorption and XRF analyses revealed that by increasing the calcination temperature from 200 to 800 °C, the Ce-LDH material transforms to ceria (CeO2) in four distinct phases, i.e., the loss of intramolecular water, dehydroxylation, removal of nitrate groups and removal of sulfate groups. When loaded with 2.5 wt% palladium (Pd) and 2.5 wt% nickel (Ni) and calcined at 500 °C, the PdNi-Ce-LDH-derived catalysts strongly outperform the PdNi-CeO2 benchmark catalyst in terms of conversion as well as selectivity for the hydrogenolysis of benzyl phenyl ether (BPE), a model compound for the ?-O-4 ether linkage in lignin. The PdNi-Ce-LDH catalysts showed full selectivity towards phenol and toluene while the PdNi-CeO2 catalysts showed additional oxidation of toluene to benzoic acid. The highest BPE conversion was observed with the PdNi-Ce-LDH catalyst calcined at 600 °C, which could be related to an optimum in morphological and compositional characteristics of the support.
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Project description:Arenes are widely used chemicals and essential components in liquid fuels, which are currently produced from fossil feedstocks. Here, we proposed the self-supported hydrogenolysis (SSH) of aromatic ethers to produce arenes using the hydrogen source within the reactants, and it was found that RuW alloy nanoparticles were very efficient catalyst for the reactions. This route is very attractive and distinguished from the reported studies on the cleavage of the CAr?O bonds. The unique feature of this methodology is that exogenous hydrogen or other reductant is not required, and hydrogenation of aromatic rings could be avoided completely. The selectivities to arenes could reach >99.9% at complete conversion of the ethers. Moreover, lignin could also be transformed into arenes efficiently over the RuW alloy catalyst. The mechanism studies showed that the neighboring Ru and W species in the RuW alloy nanoparticles worked synergistically to accelerate the SSH reaction.
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2019-01-01 | S-EPMC6648438 | BioStudies
Project description:Direct C-O hydrogenolysis of bioglycerine to produce 1,3-propanediol selectively is a vital technology that can expand the scope of biodiesel industry and green chemical production from biomass. Herein we report sulphuric acid-activated montmorillonite clay supported platinum nanoparticles as highly effective solid acid catalysts for the selective production of 1,3-propanediol from glycerol. The catalytic performances of the catalysts were investigated in the hydrogenolysis of glycerol with a fixed bed reactor under ambient pressure. The results were found promising and showed that the activation of montmorillonite by sulphuric acid incorporated Brønsted acidity in the catalyst and significantly improved the selectivity to 1,3-propanediol. The catalytic performance of different platinum loaded catalysts was examined and 2?wt% Pt/S-MMT catalyst presented superior activity among others validating 62% 1,3-propanediol selectivity at 94% glycerol conversion. The catalytic activity of 2Pt/S-MMT was systematically investigated under varying reaction parameters including reaction temperature, hydrogen flow rate, glycerol concentration, weight hourly space velocity, and contact time to derive the optimum conditions for the reaction. The catalyst stability, reusability and structure-activity correlation were also elucidated. The high performance of the catalyst could be ascribed to well disperse Pt nanoparticles immobilized on acid-activated montmorillonite, wider pore-structure and appropriate acid sites of the catalyst.
2018-01-01 | S-EPMC5945670 | BioStudies
Project description:C-lignin is a homo-biopolymer, being made up of caffeyl alcohol exclusively. There is significant interest in developing efficient and selective catalyst for depolymerization of C-lignin, as it represents an ideal feedstock for producing catechol derivatives. Here we report an atomically dispersed Ru catalyst, which can serve as an efficient catalyst for the hydrogenolysis of C-lignin via the cleavage of C-O bonds in benzodioxane linkages, giving catechols in high yields with TONs up to 345. A unique selectivity to propenylcatechol (77%) is obtained, which is otherwise hard to achieve, because this catalyst is capable of hydrogenolysis rather than hydrogenation. This catalyst also demonstrates good reusability in C-lignin depolymerization. Detailed investigations by model compounds concluded that the pathways involving dehydration and/or dehydrogenation reactions are incompatible routes; we deduced that caffeyl alcohol generated via concurrent C-O bonds cleavage of benzodioxane unit may act as an intermediate in the C-lignin hydrogenolysis. Current demonstration validates that atomically dispersed metals can not only catalyze small molecules reactions, but also drive the transformation of abundant and renewable biopolymer.
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Project description:UNLABELLED: BACKGROUND: While the ethanol production from biomass by consolidated bioprocess (CBP) is considered to be the most ideal process, simultaneous saccharification and fermentation (SSF) is the most appropriate strategy in practice. In this study, one-pot bioethanol production, including cellulase production, saccharification of cellulose, and ethanol production, was investigated for the conversion of biomass to biofuel by co-culture of two different microorganisms such as a hyper cellulase producer, Acremonium cellulolyticus C-1 and an ethanol producer Saccharomyces cerevisiae. Furthermore, the operational conditions of the one-pot process were evaluated for maximizing ethanol concentration from cellulose in a single reactor. RESULTS: Ethanol production from cellulose was carried out in one-pot bioethanol production process. A. cellulolyticus C-1 and S. cerevisiae were co-cultured in a single reactor. Cellulase producing-medium supplemented with 2.5 g/l of yeast extract was used for productions of both cellulase and ethanol. Cellulase production was achieved by A. cellulolyticus C-1 using Solka-Floc (SF) as a cellulase-inducing substrate. Subsequently, ethanol was produced with addition of both 10%(v/v) of S. cerevisiae inoculum and SF at the culture time of 60 h. Dissolved oxygen levels were adjusted at higher than 20% during cellulase producing phase and at lower than 10% during ethanol producing phase. Cellulase activity remained 8-12 FPU/ml throughout the one-pot process. When 50-300 g SF/l was used in 500 ml Erlenmeyer flask scale, the ethanol concentration and yield based on initial SF were as 8.7-46.3 g/l and 0.15-0.18 (g ethanol/g SF), respectively. In 3-l fermentor with 50-300 g SF/l, the ethanol concentration and yield were 9.5-35.1 g/l with their yields of 0.12-0.19 (g/g) respectively, demonstrating that the one-pot bioethanol production is a reproducible process in a scale-up bioconversion of cellulose to ethanol. CONCLUSION: A. cellulolyticus cells produce cellulase using SF. Subsequently, the produced cellulase saccharifies the SF, and then liberated reducing sugars are converted to ethanol by S. cerevisiae. These reactions were carried out in the one-pot process with two different microorganisms in a single reactor, which does require neither an addition of extraneous cellulase nor any pretreatment of cellulose. Collectively, the one-pot bioethanol production process with two different microorganisms could be an alternative strategy for a practical bioethanol production using biomass.
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