Lignocellulosic biomass is an abundant and renewable resource for the production of biobased value‐added fuels, chemicals, and materials, but its effective exploitation by an energy‐efficient and environmentally friendly strategy remains a challenge. Herein, a facile approach for efficiently cleaving lignin–carbohydrate complexes and ultrafast fractionation of components from wood by microwave‐assisted treatment with deep eutectic solvent is reported. The solvent was composed of sustainable choline chloride and oxalic acid dihydrate, and showed a hydrogen‐bond acidity of 1.31. Efficient fractionation of lignocellulose with the solvent was realized by heating at 80 °C under 800 W microwave irradiation for 3 min. The extracted lignin showed a low molecular weight of 913, a low polydispersity of 1.25, and consisted of lignin oligomers with high purity (ca. 96 %), and thus shows potential in downstream production of aromatic chemicals. The other dissolved matter mainly comprised glucose, xylose, and hydroxymethylfurfural. The undissolved material was cellulose with crystal I structure and a crystallinity of approximately 75 %, which can be used for fabricating nanocellulose. Therefore, this work promotes an ultrafast lignin‐first biorefinery approach while simultaneously keeping the undissolved cellulose available for further utilization. This work is expected to contribute to improving the economics of overall biorefining of lignocellulosic biomass.
Cellulose nanofibers (CNFs) were isolated from four kinds of plant cellulose fibers by a chemical-ultrasonic treatment. The chemical composition, morphology, crystalline behavior, and thermal properties of the nanofibers and their intermediate products were characterized and compared. The CNFs extracted from wood, bamboo, and wheat straw fibers had uniform diameters of 10-40 nm, whereas the flax fibers were not uniformly nanofibrillated because of their initially high cellulose content. The chemical composition of each kind of nanofibers was mainly cellulose because hemicelluloses and lignin were significantly removed during chemical process. The crystallinity of the nanofibers increased as the chemical treatments were applied. The degradation temperature of each kind of nanofiber reached beyond 330°C. Based on the properties of the CNFs, we expect that they will be suitable for use in green nanocomposites, filtration media and optically transparent films.
This article describes the fabrication of nanocellulose fibers (NCFs) with different morphologies and surface properties from biomass resources as well as their self-aggregation into lightweight aerogels. By carefully modulating the nanofibrillation process, four types of NCFs could be readily fabricated, including long aggregated nanofiber bundles, long individualized nanofibers with surface C6 -carboxylate groups, short aggregated nanofibers, and short individualized nanofibers with surface sulfate groups. Free-standing lightweight aerogels were obtained from the corresponding aqueous NCF suspensions through freeze-drying. The structure of the aerogels could be controlled by manipulating the type of NCFs and the concentration of their suspensions. A possible mechanism for the self-aggregation of NCFs into two- or three-dimensional aerogel nanostructures was further proposed. Owing to web-like structure, high porosity, and high surface reactivity, the NCF aerogels exhibited high mechanical flexibility and ductility, and excellent properties for water uptake, removal of dye pollutants, and the use as thermal insulation materials. The aerogels also displayed sound-adsorption capability at high frequencies.
With the aid of DFT calculation, deep eutectic solvents can be designed more powerful for the pretreatment of lignocellulose and the production of biochemicals.
Recent improvements in flexible electronics have increased the need to develop flexible and lightweight power sources. However, current flexible electrodes are limited by low capacitance, poor mechanical properties, and lack of cycling stability. In this article, we describe an ionic liquid-processed supramolecular assembly of cellulose and 3,4-ethylenedioxythiophene for the formation of a flexible and conductive cellulose/poly(3,4-ethylenedioxythiophene) PEDOT:poly(styrene sulfonate) (PSS) composite matrix. On this base, multiwalled carbon nanotubes (MWCNTs) were incorporated into the matrix to fabricate an MWCNT-reinforced cellulose/PEDOT:PSS film (MCPP), which exhibited favorable flexibility and conductivity. The MCPP-based electrode displayed comprehensively excellent electrochemical properties, such as a low resistance of 0.45 Ω, a high specific capacitance of 485 F g at 1 A g, and good cycling stability, with a capacity retention of 95% after 2000 cycles at 2 A g. An MCPP-based symmetric solid-state supercapacitor with Ni foam as the current collector and PVA/KOH gel as the electrolyte exhibited a specific capacitance of 380 F g at 0.25 A g and achieved a maximum energy density of 13.2 Wh kg (0.25 A g) with a power density of 0.126 kW kg or an energy density of 4.86 Wh kg at 10 A g, corresponding to a high power density of 4.99 kW kg. Another kind of MCPP-based solid-state supercapacitor without the Ni foam showed excellent flexibility and a high volumetric capacitance of 50.4 F cm at 0.05 A cm. Both the electrodes and the supercapacitors were environmentally stable and could be operated under remarkable deformation or high temperature without damage to their structural integrity or a significant decrease in capacitive performance. Overall, this work provides a strategy for the fabrication of flexible and conductive energy-storage films with ionic liquid-processed cellulose as a medium.
A flexible, transparent, and renewable mesoporous cellulose membrane (mCel‐membrane) featuring uniform mesopores of ≈24.7 nm and high porosity of 71.78% is prepared via a facile and scalable solution‐phase inversion process. KOH‐saturated mCel‐membrane as a polymer electrolyte demonstrates a high electrolyte retention of 451.2 wt%, a high ionic conductivity of 0.325 S cm−1, and excellent mechanical flexibility and robustness. A solid‐state electric double layer capacitor (EDLC) using activated carbon as electrodes, the KOH‐saturated mCel‐membrane as a polymer electrolyte exhibits a high capacitance of 110 F g−1 at 1.0 A g−1, and long cycling life of 10 000 cycles with 84.7% capacitance retention. Moreover, a highly integrated planar‐type micro‐supercapacitor (MSC) can be facilely fabricated by directly depositing the electrode materials on the mCel‐membrane‐based polymer electrolyte without using complicated devices. The resulting MSC exhibits a high areal capacitance of 153.34 mF cm−2 and volumetric capacitance of 191.66 F cm−3 at 10 mV s−1, representing one of the highest values among all carbon‐based MSC devices. These findings suggest that the developed renewable, flexible, mesoporous cellulose membrane holds great promise in the practical applications of flexible, solid‐state, portable energy storage devices that are not limited to supercapacitors.
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