60 research outputs found

    Influence of Carbohydrates Covalently Bonded with Lignin on Solvent Fractionation, Thermal Properties, and Nanoparticle Formation of Lignin

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    The valorization of industrial lignin essentially requires fractionation resulting in lower structural heterogeneity and polydispersity. So far, extensive fractionation approaches based on extraction with solvents, gradient acid precipitation, and membrane-based filtration have been developed to reduce the polydispersity and heterogeneity of technical lignins. However, most reports tend to overlook the lignin fraction that bonded with carbohydrates or the so-called lignin carbohydrate complex (LCC), which always coexists in the initial lignin sample and can significantly affect the properties of lignin, including its homogeneity and solubility. In this study, we evaluated the ability of 13 organic solvents to separate lignin bonded with carbohydrates. It was found that carbohydrates could only be detected when the hydrogen bonding capacity (δH) of solvent was no less than 8.0 (the δH of tetrahydrofuran, THF). Based on this result, eight lignin fractions with trace/large amounts of carbohydrates and decreased heterogeneity were obtained using an elaborate sequential solvent extraction approach. The following properties of each lignin fraction were compared: elemental composition, carbohydrate content, molar mass, hydroxyl group content, and thermal properties. In addition, we also studied the ability of these lignin fractions to form lignin nanoparticles and confirmed that fractions with trace amounts of carbohydrates were able to form uniform spherical lignin nanoparticles (LNPs) than those with large amounts of carbohydrates bonded fractions. In short, this study provided a profound understanding of the role of the carbohydrates bonded to lignin on the fractionation of lignin by organic solvents, further demonstrating how carbohydrates influence the characteristics of lignin.</p

    Supercritical fluid extraction of Eucalyptus globulus bark: a promising approach for triterpenoid production

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    Eucalyptus bark contains significant amounts of triterpenoids with demonstrated bioactivity, namely triterpenic acids and their acetyl derivatives (ursolic, betulinic, oleanolic, betulonic, 3-acetylursolic, and 3-acetyloleanolic acids). In this work, the supercritical fluid extraction (SFE) of Eucalyptus globulus deciduous bark was carried out with pure and modified carbon dioxide to recover this fraction, and the results were compared with those obtained by Soxhlet extraction with dichloromethane. The effects of pressure (100-200 bar), co-solvent (ethanol) content (0, 5 and 8% wt), and multistep operation were studied in order to evaluate the applicability of SFE for their selective and efficient production. The individual extraction curves of the main families of compounds were measured, and the extracts analyzed by GC-MS. Results pointed out the influence of pressure and the important role played by the co-solvent. Ethanol can be used with advantage, since its effect is more important than increasing pressure by several tens of bar. At 160 bar and 40 degrees C, the introduction of 8% (wt) of ethanol greatly improves the yield of triterpenoids more than threefold

    Expression of fungal acetyl xylan esterase in Arabidopsis thaliana improves saccharification of stem lignocellulose

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    Cell wall hemicelluloses and pectins are O-acetylated at specific positions, but the significance of these substitutions is poorly understood. Using a transgenic approach, we investigated how reducing the extent of O-acetylation in xylan affects cell wall chemistry, plant performance and the recalcitrance of lignocellulose to saccharification. The Aspergillus niger acetyl xylan esterase AnAXE1 was expressed in Arabidopsis under the control of either the constitutively expressed 35S CAMV promoter or a woody-tissue-specific GT43B aspen promoter, and the protein was targeted to the apoplast by its native signal peptide, resulting in elevated acetyl esterase activity in soluble and wall-bound protein extracts and reduced xylan acetylation. No significant alterations in cell wall composition were observed in the transgenic lines, but their xylans were more easily digested by a beta-1,4-endoxylanase, and more readily extracted by hot water, acids or alkali. Enzymatic saccharification of lignocellulose after hot water and alkali pretreatments produced up to 20% more reducing sugars in several lines. Fermentation by Trametes versicolor of tissue hydrolysates from the line with a 30% reduction in acetyl content yielded similar to 70% more ethanol compared with wild type. Plants expressing 35S: AnAXE1 and pGT43B:AnAXE1 developed normally and showed increased resistance to the biotrophic pathogen Hyaloperonospora arabidopsidis, probably due to constitutive activation of defence pathways. However, unintended changes in xyloglucan and pectin acetylation were only observed in 35S: AnAXE1-expressing plants. This study demonstrates that postsynthetic xylan deacetylation in woody tissues is a promising strategy for optimizing lignocellulosic biomass for biofuel production.Peer reviewe

    Non-cellulosic heteropolysaccharides from sugarcane bagasse - Sequential extraction with pressurized hot water and alkaline peroxide at different temperatures

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    The xylan-rich hemicellulose components of sugarcane bagasse were sequentially extracted with pressurized hot-water extraction (PHWE) and alkaline peroxide. The hemicelluloses were found to contain mainly arabinoxylans with varying substitutions confirmed by different chemical and spectroscopic methods. The arabinoxylans obtained from PHWE were found to be more branched compared to those obtained after alkaline extraction. Sequential extraction could be useful for the isolation of hemicelluloses with different degree of branching, molar mass, and functional groups from sugarcane bagasse, which can be of high potential use for various industrial applications

    Bio-Based Hydrogels With Ion Exchange Properties Applied to Remove Cu(II), Cr(VI), and As(V) Ions From Water

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    Hydrogels with ion exchange properties were synthesized from compounds derived from wood biopolymer hemicellulose and from commercial vinyl monomers to be tested as active materials for the removal of Cu(II), Cr(VI), and As(V) ions. The hemicellulose O-acetyl galactoglucomannan (GGM) was used as the precursor material, and through a transesterification reaction, GGM was converted into a macromonomer GGM-glycidyl methacrylate (GGM-GMA). Subsequently, the GGM-GMA macromonomer, containing more than one methacrylate group, was used as a crosslinking agent in the synthesis of hydrogels through free-radical polymerization reactions in combination with a 2-acrylamido-2-methyl-1-propanesulfonic acid monomer to produce a cation exchange hydrogel. Also, (3-acrylamidopropyl)trimethylammonium chloride monomer was applied together with the GGM-GMA to form hydrogels that can be used as anion exchange hydrogel. The hydrogels were characterized by Fourier transform-infrared (FT-IR), H-1-NMR spectroscopy, and thermogravimetric analysis (TGA), as well as derivative thermogravimetry (DTG). The microstructure of the hydrogels was characterized by scanning electron microscopy (SEM) analysis with X-ray microanalysis energy-dispersive spectroscopy (EDS). The results obtained regarding the absorption capacity of the Cu(II), Cr(VI), and As(V) ions were studied as a function of the pH value and the initial concentration of the metal ions in the solutions. Absorption was carried out in consecutive batches, and it was found that the poly(GGM-GMA/AMPSH) hydrogel reached an absorption capacity of 90 mg g(-1) for Cu(II). The poly(GGM-GMA/APTACl) hydrogel reached values of 69 and 60 mg g(-1) for Cr(VI) and As(V) oxyanions, respectively. Tests with polymer blends (mixtures of anionic and cationic hydrogels) were also carried out to remove Cu(II), Cr(VI), and As(V) ions from multi-ionic solutions, obtaining satisfactory results

    On Low-Concentration Inks Formulated by Nanocellulose Assisted with Gelatin Methacrylate (GelMA) for 3D Printing toward Wound Healing Application

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    Cellulose nanofibrils (CNFs) in the form of hydrogels stand out as a platform biomaterial in bioink formulation for 3D printing because of their low cytotoxicity and structural similarity to extracellular matrices. In the present study, 3D scaffolds were successfully printed with low-concentration inks formulated by 1 w/v % 2,2,6,6-Tetramethylpiperidine-1-oxyl radical (TEMPO)-oxidized CNF with less than 1 w/v % gelatin methacrylate (GelMA). Quartz crystal microbalance with dissipation monitoring (QCM-D) measurements showed strong interaction between the two biopolymers. The UV cross-linking ability of GelMA (≤1 w/v %) was enhanced in the presence of TEMPO-oxidized CNFs. Multiple factors including strong physical interaction between CNF and GelMA, in situ cross-linking of CNF by Ca 2+ , and UV cross-linking of GelMA enabled successful 3D printing of low-concentration inks of CNF/GelMA into scaffolds possessing good structural stability. The mechanical strength of the scaffolds was tuned in the range of 2.5 to 5 kPa. The cell culture with 3T3 fibroblasts revealed noncytotoxic and biocompatible features for the formulated inks and printed scaffolds. More importantly, the incorporated GelMA in the CNF hydrogel promoted the proliferation of fibroblasts. The developed low-concentration CNF/GelMA formulations with a facile yet effective approach to fabricate scaffolds showed great potential in 3D printing for wound healing application

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