Process Development for Flexible Films of Industrial Cellulose Pulp Using Superbase Ionic Liquids.
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ABSTRACT:
SUBMITTER: Ribeiro DCM
PROVIDER: S-EPMC8199285 | biostudies-literature |
REPOSITORIES: biostudies-literature
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Project description:ObjectivesIonic liquids (ILs) that dissolve biomass are harmful to the enzymes that degrade lignocellulose. Enzyme hyperthermostability promotes a tolerance to ILs. Therefore, the limits of hyperthemophilic Pyrococcus horikoschii endoglucanase (PhEG) to tolerate 11 superbase ILs were explored.ResultsPhEG was found to be most tolerant to 1-ethyl-3-methylimidazolium acetate ([EMIM]OAc) in soluble 1% carboxymethylcellulose (CMC) and insoluble 1% Avicel substrates. At 35% concentration, this IL caused an increase in enzyme activity (up to 1.5-fold) with CMC. Several ILs were more enzyme inhibiting with insoluble Avicel than with soluble CMC. Km increased greatly in the presence ILs, indicating significant competitive inhibition. Increased hydrophobicity of the IL cation or anion was associated with the strongest enzyme inhibition and activation. Surprisingly, PhEG activity was increased 2.0-2.5-fold by several ILs in 4% substrate. Cations exerted the main role in competitive inhibition of the enzyme as revealed by their greater binding energy to the active site.ConclusionsThese results reveal new ways to design a beneficial combination of ILs and enzymes for the hydrolysis of lignocellulose, and the strong potential of PhEG in industrial, high substrate concentrations in aqueous IL solutions.
| S-EPMC9356960 | biostudies-literature
Project description:1-(1,3-diethoxy-1,3-dioxopropan-2-ylo)-3-methylimidazolium bromide (RIL1_Br), 1-(2-etoxy-2-oxoethyl)-3-methylimidazolium bromide (RIL2_Br), 1-(2-etoxy-2-oxoethyl)-3-methylimidazolium tetrafluoroborate (RIL3_BF4) ionic liquids were synthesized. Subsequently, the dense cellulose acetate propionate (CAP)-based materials containing from 9 to 28.6 wt % of these reactive ionic liquids were elaborated. Reactive ionic liquids (RILs) were immobilized in CAP as a result of the transesterification reaction. The yield of this reaction was over 90% with respect to the used RIL. The physicochemical properties of resultant films were studied using nuclear magnetic resonance (NMR), scanning electron microscopy (SEM), energy dispersive X-ray (EDX), atomic force microscopy (AFM), and thermogravimetric analysis (TGA). The RIL incorporation influenced the morphology of films by increasing their surface roughness with the rise of RIL content. The thermal stability of CAP-based membranes was dependent on the nature of the ionic liquid. Nevertheless, it was proven that CAP films containing RILs were stable up to 120-150 °C. Transport properties were characterized by water permeation tests. It was found that the type and the amount of the ionic liquid in the CAP matrix substantially influenced the transport properties of the prepared hybrid materials.
| S-EPMC6680812 | biostudies-other
Project description:The fabrication of self-assembled cellulose nanocrystal (CNC) films of tunable photonic and mechanical properties using a facile, green approach is demonstrated. The combination of tunable flexibility and iridescence can dramatically expand CNC coating and film barrier capabilities for paints and coating applications, sustainable consumer packaging products, as well as effective templates for photonic and optoelectronic materials and structures.
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Project description:Electrode-polymer interfaces dictate many of the properties of thin films such as capacitance, the electric field experienced by polymers, and charge transport. However, structure and dynamics of charged polymers near electrodes remain poorly understood, especially in the high concentration limit representative of the melts. To develop an understanding of electric field–induced transformations of electrode-polymer interfaces, we have studied electrified interfaces of an imidazolium-based polymerized ionic liquid (PolyIL) using combinations of broadband dielectric spectroscopy, specular neutron reflectivity, and simulations based on the Rayleigh’s dissipation function formalism. Overall, we obtained the camel-shaped dependence of the capacitance on applied voltage, which originated from the responses of an adsorbed polymer layer to applied voltages. This work provides additional insights related to the effects of molecular weight in affecting structure and properties of electrode-polymer interfaces, which are essential for designing next-generation energy storage and harvesting devices.
| S-EPMC7319767 | biostudies-literature
Project description:Forestry industries in Chile are facing an important challenge-diversifying their products using green technologies. In this study, the potential use of Ionic Liquids (ILs) to dissolve and hydrolyze eucalyptus wood (mix of Eucalyptus nitens and Eucalyptus globulus) kraft pulp was studied. The Bleached Hardwood Kraft Pulp (BHKP) from a Chilean pulp mill was used together with five different ILs: 1-butyl-3-methylimidazolium chloride [bmim][Cl], 1-butyl-3-methylimidazolium acetate [bmim][Ac], 1-butyl-3-methylimidazolium hydrogen sulfate [bmim][HSO4], 1-ethyl-3-methylimidazolium chloride [emim][Cl], 1-ethyl-3-methylimidazolium acetate [emim][Ac]. Experimentally, one vacuum reactor was designed to study the dissolution/hydrolysis process for each ILs; particularly, the cellulose dissolution process using [bmim][Cl] was studied proposing one molecular dynamic model. Experimental characterization using Atomic Force Microscopy, conductometric titration, among other techniques suggest that all ILs are capable of cellulose dissolution at different levels; in some cases, the dissolution evolved to partial hydrolysis appearing cellulose nanocrystals (CNC) in the form of spherical aggregates with a diameter of 40-120 nm. Molecular dynamics simulations showed that the [bmim][Cl] anions tend to interact actively with cellulose sites and water molecules in the dissolution process. The results showed the potential of some ILs to dissolve/hydrolyze the cellulose from Chilean Eucalyptus, maintaining reactive forms.
| S-EPMC6523854 | biostudies-other
Project description:Cellulose from cotton fibers was functionalized through a dissolution-regeneration process with phosphonate-based ionic liquids (ILs): 1,3-dimethylimidazolium methylphosphonate [DIMIM][(MeO)(H)PO2] and 1-ethyl-3-methylimidazolium methylphoshonate [EMIM][(MeO)(H)PO2]. The chemical modification of cellulose occurred through a transesterification reaction between the methyl phosphonate function of ILs and the primary alcohol functions of cellulose. The resulting cellulose structure and the amount of grafted phosphorus were then investigated by X-ray diffraction, ICP-AES, and ¹³C and ³¹P NMR spectroscopy. Depending on the IL type and initial cotton / IL ratio in the solution, regenerated cellulose contained up to 4.5% of phosphorus. The rheological behavior of cotton cellulose/ILs solutions and the microscale fire performances of modified cellulose were studied in order to ultimately prepare flame retardant cellulosic materials. Significant improvement in the flame retardancy of regenerated cellulose was obtained with a reduction of THR values down to about 5-6 kJ/g and an increase of char up to about 35 wt%.
| S-EPMC7181116 | biostudies-literature
Project description:This study investigates flexible (polyamide 6.6 PA-6.6, polyethylene terephthalate PET, Cu, Al, and Ni foils) and, for comparison, stiff substrates (silicon wafers and glass) differing in, for example, in surface free energy and surface roughness and their ability to host cellulose-based thin films. Trimethylsilyl cellulose (TMSC), a hydrophobic acid-labile cellulose derivative, was deposited on these substrates and subjected to spin coating. For all the synthetic polymer and metal substrates, rather homogenous films were obtained, where the thickness and the roughness of the films correlated with the substrate roughness and its surface free energy. A particular case was the TMSC layer on the copper foil, which exhibited superhydrophobicity caused by the microstructuring of the copper substrate. After the investigation of TMSC film formation, the conversion to cellulose using acidic vapors of HCl was attempted. While for the polymer foils, as well as for glass and silicon, rather homogenous and smooth cellulose films were obtained, for the metal foils, there is a competing reaction between the formation of metal chlorides and the generation of cellulose. We observed particles corresponding to the metal chlorides, while we could not detect any cellulose thin films after HCl treatment of the metal foils as proven by cross-section imaging using scanning electron microscopy (SEM).
| S-EPMC6316936 | biostudies-literature
Project description:Ethyl cellulose was grafted with ionic liquids in optimal yields (62.5-64.1%) and grafting degrees (5.93-7.90%) by the esterification of the hydroxyl groups in ethyl cellulose with the carboxyl groups in ionic liquids. In IR spectra of the ethyl cellulose derivatives exhibited C=O bond stretching vibration peaks at 1760 or 1740 cm-1, confirming the formation of the ester groups and furnishing the evidence of the successful grafting of ethyl cellulose with ionic liquids. The ethyl cellulose grafted with ionic liquids could be formed into membranes by using the casting solution method. The resulting membranes exhibited good membrane forming ability and mechanical properties. The EC grafted with ionic liquids-based membranes demonstrated PCO2/PCH4 separation factors of up to 18.8, whereas the PCO2/PCH4 separation factor of 9.0 was obtained for pure EC membrane (both for CO2/CH4 mixture gas). The membranes also demonstrated an excellent gas permeability coefficient PCO2, up to 199 Barrer, which was higher than pure EC (PCO2 = 46.8 Barrer). Therefore, it can be concluded that the ionic liquids with imidazole groups are immensely useful for improving the gas separation performances of EC membranes.
| S-EPMC6918432 | biostudies-literature
Project description:Ionic Liquids are a broad group of salts with low melting points that can be specifically tuned for a broad range of applications. Despite being initially considered “green” solvents, their better environmental friendliness compared to traditional solvents has been increasingly challenged. In this study, we aimed to investigate the molecular effects of ILs exposure by using RNA-sequencing to study differential gene expression patterns. Thus, we exposed Daphnia magna to 1-ethyl-3-methylimidazolium chloride ([C2mim]Cl), 1-dodecyl chloride-3-methylimidazolium ([C12mim]Cl) and cholinium chloride ([Chol]Cl). Results suggest that the three ILs share several mechanisms of toxicity, including cellular membrane and cytoskeleton damage, oxidative stress, inhibition of antioxidant enzymes, mitochondrial affectation, changes in protein biosynthesis and energy production, DNA damage, and ultimately, programmed cell death and disease initiation. Overall, the dataset revealed that [C2mim]Cl and [C12mim]Cl were, respectively, the least and the most toxic ILs at the transcriptional level. Also, it is reinforced that [Chol]Cl is not devoid of environmental hazardous potential. Unique gene expression signatures could also be identified for each IL.
2021-08-13 | GSE156769 | GEO
Project description:We present 1,2,3-triazolium- and imidazolium-based ionic liquids (ILs) with aromatic anions as a new class of cellulose solvents. The two anions in our study, benzoate and salicylate, possess a lower basicity when compared to acetate and therefore should lead to a lower amount of N-heterocyclic carbenes (NHCs) in the ILs. We characterize their physicochemical properties and find that all of them are liquids at room temperature. By applying force field molecular dynamics (MD) simulations, we investigate the structure and dynamics of the liquids and find strong and long-lived hydrogen bonds, as well as significant ?-? stacking between the aromatic anion and cation. Our ILs dissolve up to 8.5 wt.-% cellulose. Via NMR spectroscopy of the solution, we rule out chain degradation or derivatization, even after several weeks at elevated temperature. Based on our MD simulations, we estimate the enthalpy of solvation and derive a simple model for semi-quantitative prediction of cellulose solubility in ILs. With the help of Sankey diagrams, we illustrate the hydrogen bond network topology of the solutions, which is characterized by competing hydrogen bond donors and acceptors. The hydrogen bonds between cellulose and the anions possess average lifetimes in the nanosecond range, which is longer than found in common pure ILs.
| S-EPMC7435399 | biostudies-literature