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Recent advancements in metal-organic frameworks (MOFs) underscore their significant potential in chemical and materials research, owing to their remarkable properties and diverse structures. Despite challenges like intrinsic brittleness, powdered crystalline nature, and limited stability impeding direct applications, MOF-based aerogels have shown superior performance in various areas, particularly in water treatment and contaminant removal. This review highlights the latest progress in MOF-based aerogels, with a focus on hybrid systems incorporating materials like graphene, carbon nanotube, silica, and cellulose in MOF aerogels, which enhance their functional properties. The manifold advantages of MOF-based aerogels in energy storage, adsorption, and catalysis are discussed, with an emphasizing on their improved stability, processability, and ease of handling. This review aims to unlock the potential of MOF-based aerogels and their real-world applications. Aerogels are expected to reshape the technological landscape of MOFs through enhanced stability, adaptability, and efficiency.
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We study the effect of electrolytes on the stability in aqueous media of spherical lignin particles (LP) and its relevance to Pickering emulsion stabilization. Factors considered included the role of ionic strength on morphology development, LP size distribution, surface charge, interfacial adsorption, colloidal and wetting behaviors. Stable emulsions are formed at salt concentrations as low as 50 mM, with the highest stability observed at a critical concentration (400 mM). We show salt-induced destabilization of LP aqueous dispersions at an ionic strength >400 mM. At this critical concentration LP flocculation takes place and particulate networks are formed. This has a profound consequence on the stability of LP-stabilized Pickering emulsions, affecting rheology and long-term stability. The results along with quartz microgravimetry and confocal microscopy observations suggest a possible mechanism for stabilization that considers the interfacial adsorption of LP at oil/water interfaces. The often-unwanted colloidal LP destabilization in water ensues remarkably stable Pickering emulsions by the effect of network formation.
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Coloides , Emulsiones , Lignina , Agua , Emulsiones/química , Lignina/química , Coloides/química , Agua/química , Floculación , Concentración Osmolar , Adsorción , Sales (Química)/química , Reología , Tamaño de la PartículaRESUMEN
Supercapacitors are the preferred option for supporting renewable energy sources owing to many benefits, including fast charging, long life, high energy and power density, and saving energy. While electrode materials with environmentally friendly preparation, high performance, and low cost are important research directions of supercapacitors. At present, the growing global population and the increasingly pressing issue of environmental pollution have drawn the focus of numerous researchers worldwide to the development and utilization of renewable biomass resources. Lignin, a renewable aromatic polymer, has reserves second only to cellulose in nature. Ten million tonnes of industrial lignin are produced in pulp and paper mills annually, most of which are disposed of as waste or burned for fuel, seriously depleting natural resources and polluting the environment. One practical strategy to accomplish sustainable development is to employ lignin resources to create high-value materials. Based on the high carbon content and rich functional groups of lignin, the lignin-based carbon materials generated after carbonization treatment display specific electrochemical properties as electrode materials. Nevertheless, low electrochemical activity of untreated lignin precludes it from achieving its full potential for application in energy storage. Heteroatom doping is a common modification method that aims to improve the electrochemical performance of the electrode materials by optimizing the structure of the lignin, improving its pore structure and increasing the number of active sites on its surface. This paper aims to establish theoretical foundations for design, preparation, and optimizing the performance of heteroatom-doped lignin-based carbon materials, as well as for developing high-value-added lignin materials. The most reported the mechanism of supercapacitors, the doping process involving various types of heteroatoms, and the analysis of how heteroatoms affect the performance of lignin-based carbon materials are also detailed in this review.
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Carbono , Capacidad Eléctrica , Electrodos , Lignina , Lignina/química , Carbono/químicaRESUMEN
Cellulose, hemicellulose, and lignin are the major bio-components in lignocellulosic biomass (BC-LB), which possess excellent biomechanical properties and biocompatibility to satisfy the demands of orthopedic applications. To understand the basis and trends in the development of major bio-components in BC-LB in orthopedics, the bibliometric technology was applied to get unique insights based on the published papers (741) in the Web of Science (WOS) database from January 1st, 2001, to February 14th, 2023. The analysis includes the annual distributions of publications, keywords co-linearity, research hotspots exploration, author collaboration networks, published journals, and clustering of co-cited literature. The results reveal a steady growth in publications focusing on the application of BC-LB in orthopedics, with China and the United States leading in research output. The "International Journal of Biological Macromolecules" was identified as the most cited journal for BC-LB research in orthopedics. The research hotspots encompassed bone tissue engineering, cartilage tissue engineering, and drug delivery systems, indicating the fundamental research and potential development in these areas. This study also highlights the challenges associated with the clinical application of BC-LB in orthopedics and provides valuable insights for future advancements in the field.
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Bibliometría , Biomasa , Celulosa , Lignina , Ortopedia , Polisacáridos , Lignina/química , Polisacáridos/química , Celulosa/química , Humanos , Ingeniería de Tejidos/métodosRESUMEN
In this work, new N, O-codoped chitosan-derived carbon adsorbents (CKC-x, x refer to the calcination temperature) were synthesized over a simple process of chitosan-KOH aerogel production and simultaneous carbonization/activation of the aerogel. CKC-700 was characterized by sheet-like morphology (even containing a portion of carbon nano-sheet of 3 nm thickness), high porosity and specific surface area (1702.1 m2/g), and pyridinic/pyrrolic/graphitic N groups. The simultaneous carbonization/activation of chitosan-KOH aerogel prepared by top-down coagulation of chitosan aqueous solution by KOH aqueous solution rendered these beneficial characteristics. CKC-700 exhibited a superior adsorption capacity for Rhodamine B (RhB) to other chitosan-derived carbon adsorbents, and the maximum adsorption capacity for RhB of 594 mg/g was achieved at 55 °C. CKC-700 also possessed reasonable reusability for the removal of RhB, and the removal efficiency was still above 95 % in the fifth cycle. The effects of adsorption temperature and time, adsorbent dose, organic dye concentration, and solution pH on the adsorption capacity of CKC-700 were studied. Moreover, the adsorption isotherm, kinetics, thermodynamics, and the adsorption mechanism of RhB on CKC-700 were discussed. In addition, CKC-700 also showed favorable adsorption performance for methylene blue (441 mg/g), methyl orange (457 mg/g), and congo red (500 mg/g) at around 25 °C.
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Hydroxypropyl cellulose (HPC) is a sustainable cellulose derivative valued for its excellent biocompatibility and solubility and is widely used in various fields. Recent scientific research on high-substituted HPC mainly focused on its efficient preparation and phase transition behavior. Herein, a novel strategy of high-substituted HPC synthesis was demonstrated by employing DMSO/TBAF·3H2O as a cellulose solvent, exhibiting more efficiency than traditional approaches. High-substituted HPC prepared has remarkable thermal stability, exceptional hydrophilicity, and satisfactory solubility. Phase transition behavior of HPC with varying molar degrees of substitution (MS) was delved and a notable negative correlation between MS and cloud point temperature (TCP), was revealed, particularly evident at an MS of 12.3, where the TCP drops to 33 °C. Moreover, a unique self-assembly behavior featuring structural color and responsiveness to force in a solvent-free environment emerged when the MS exceeded 10.4. These insights comprehensively strengthen the understanding and knowledge of high-substituted HPC, simultaneously paving the way for further HPC investigation and exploitation.
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Lignin, as an abundant aromatic biopolymer in plants, has great potential for medical applications due to its active sites, antioxidant activity, low biotoxicity, and good biocompatibility. In this work, a simple and ecofriendly approach for lignin fractionation and modification was developed to improve the antitumor activity of lignin. The lignin fraction KL-3 obtained by the lignin gradient acid precipitation at pH = 9-13 showed good cytotoxicity. Furthermore, the cell-feeding lignin after additional structural modifications such as demethylation (DKL-3), sulfonation (SL-3), and demethylsulfonation (DSKL-3) could exhibit higher glutathione responsiveness in the tumor microenvironment, resulting in reactive oxygen species accumulation and mitochondrial damage and eventually leading to apoptosis in HepG2 cells with minimal damage to normal cells. The IC50 values for KL-3, SL-3, and DSKL-3 were 0.71, 0.57, and 0.41 mg/mL, respectively, which were superior to those of other biomass extractives or unmodified lignin. Importantly, in vivo experiments conducted in nude mouse models demonstrated good biosafety and effective tumor destruction. This work provides a promising example of constructing carrier-free functionalized lignin antitumor materials with different structures for inhibiting the growth of human hepatocellular carcinoma (HepG2) cells, which is expected to improve cancer therapy outcomes.
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Carcinoma Hepatocelular , Neoplasias Hepáticas , Poliuretanos , Animales , Ratones , Humanos , Carcinoma Hepatocelular/tratamiento farmacológico , Carcinoma Hepatocelular/patología , Neoplasias Hepáticas/tratamiento farmacológico , Neoplasias Hepáticas/patología , Células Hep G2 , Lignina/farmacología , Microambiente TumoralRESUMEN
Petroleum-based plastics are useful but they pose a great threat to the environment and human health. It is highly desirable yet challenging to develop sustainable structural materials with excellent mechanical and optical properties for plastic replacement. Here, we report a simple and efficient method to manufacture high-performance all-biobased structural materials from cellulosic wood skeleton (WS) and gelatin via oxidation and densification. Specifically, gelatin was grafted to the oxidized cellulose wood skeletons (DAWS) and then physically crosslinked via Tannic acid (TA), resulting in a significant enhancement of the material properties. Notably, only a mild pressure was applied during the drying process to form a densified TA/Gelatin/transparent wood film(TWF). The developed TA/Gelatin/TWF (thickness:100 ± 12 µm) exhibited a desirable combination of high strength (â¼154.59 MPa), light transmittance (86.2 % at 600 nm), low haze (16.7 %), high water stability (wet strength: â¼130.13 MPa) and ultraviolet blocking efficacy which surpass most of the petroleum-based plastics. In addition, due to the all bio-based origins (wood and gelatin), TA/Gelatin/TWF are easily biodegradable under natural conditions, leading to less impact on the environment. These findings would hold promises for exploring high-quality all bio-based wood composites as eco-friendly alternatives to substitute plastics with wide applications, e.g. anti-counterfeiting, UV protection, and flexible electricals.
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Celulosa Oxidada , Petróleo , Humanos , Gelatina , MaderaRESUMEN
Lignin is the most abundant aromatic biomass resource in nature and is the main by-product of paper industry and biorefinery industry, which has the characteristics of abundant source, renewable and low cost. Deep eutectic solvents (DES) are a nascent environmentally friendly solvent option that is gaining traction. DES composed of p-toluenesulfonic acid and choline chloride is used for batch treatment of alkaline lignin, and the bio-oil obtained is ternary polymerized with formaldehyde and phenol to obtain lignin phenolic resin. The porous carbon material is produced through a two-step carbonization process, utilizing phenolic resin derived from lignin as the primary source of carbon. The morphology and composition of the carbon were analyzed by SEM, TEM, XRD, TGA, XPS and Raman spectroscopy, the specific surface area and pore size distribution were analyzed by BET. The results showed that the specific surface area of the lignin-based phenolic resin was significantly higher than that of the pure phenolic resin carbon, and the porous carbon material that was acquired demonstrated a specific surface area of as much as 1026 m2/g. In the three-electrode system, the specific capacitance of DLPFC can reach 245.8 F/g (0.25 A/g), with a very small decrease in the value of specific capacitance at 10,000 cycles, with a retention of 97.62% (10 A/g). The porous carbon demonstrated a specific capacitance of 112.4 F/g at a current density of 0.5 A/g, and the capacitance retention rate could still reach 98.8% after 5000 charge/discharge cycles, with high cycling stability (in the two-electrode system). The prepared symmetrical supercapacitors exhibited high energy density and power density of 3.9 Wh/kg and 125.0 W/kg. The results suggest a new idea of high value-added application of lignin phenolic resin for high-performance supercapacitor electrodes.
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Carbono , Lignina , Lignina/química , Carbono/química , Porosidad , Fenoles , Formaldehído , ElectrodosRESUMEN
To screen and evaluate excellent blackberry cultivars and strains, 17 indexes of plant growth and fruit horticultural and nutritional characteristics were measured, 20 simple sequence repeat (SSR) markers were analyzed, the fingerprints of 23 blackberry cultivars and strains were constructed, and the processing characteristics of 10 excellent cultivars and strains were evaluated. The results showed that 'Chester' and 'Shuofeng' had the highest plant yield (6.5 kg per plant), of which the 'Chester' fruit also had the highest hardness (2.78 kg/cm2). 'Kiowa' had the highest single fruit weight (10.43 g). '10-5n-2' had the highest total anthocyanin content (225.4 mg/100 g FW) and total polyphenol content (3.24 mg/g FW), but a low plant yield. These results suggest that 'Shuofeng' and 'Chester' are the top two blackberry cultivars planted in Nanjing, with the best growth and comprehensive quality. Moreover, a total of 119 alleles were detected with an average number of 6 alleles per locus. The polymorphism information content (PIC) was 0.374~0.844, with an average of 0.739, indicating a high genetic diversity among the 23 blackberry cultivars and strains. This study provides insight into the plant growth, fruit characteristics and genetic diversity of the 23 blackberry cultivars and strains, and is thus conducive to the protection and utilization of blackberry cultivars and strains.
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Multistimuli-responsive fluorescent materials have garnered great research interest benefited from their practical applications. Two twisted-structure compounds containing tetraphenylethylene (TPE) as the aggregation-induced emission (AIE) group and a pyridine unit as the acid reaction site to obtain new multistimuli-responsive fluorescent compounds (namely, TPECNPy: TPECNPy-2 and TPECNPy-3) were successfully synthesized through a one-step Knoevenagel condensation reaction. The multiple-stimuli response process of TPECNPy was investigated by means of photoluminescence (PL) spectra and emission colour. The results showed that both TPECNPy compounds with excellent AIE abilities displayed reversible emission wavelength and colour changes in response to multiple external stimuli, including grinding-fuming by CH2 Cl2 or annealing and HCl-NH3 vapour fuming. More importantly, fluorescent nanofibre films were prepared by electrospinning a solution of TPECNPy mixed with cellulose acetate (CA), and these exhibited reversible acid-induced discolouration, even with only 1 wt% TPECNPy. The results of this study may inspire strategies for designing multistimuli-responsive materials and preparing fluorescent sensing nanofibre films.
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Nanofibras , Fluorescencia , Colorantes Fluorescentes/químicaRESUMEN
Polysaccharides, due to their remarkable features, have gained significant prominence in the sustainable production of nanoparticles (NPs). High market demand and minimal production cost, compared to the chemically synthesised NPs, demonstrate a drive towards polysaccharide-based nanoparticles (PSNPs) benign to environment. Various approaches are used for the synthesis of PSNPs including cross-linking, polyelectrolyte complexation, and self-assembly. PSNPs have the potential to replace a wide diversity of chemical-based agents within the food, health, medical and pharmacy sectors. Nevertheless, the considerable challenges associated with optimising the characteristics of PSNPs to meet specific targeting applications are of utmost importance. This review provides a detailed compilation of recent accomplishments in the synthesis of PSNPs, the fundamental principles and critical factors that govern their rational fabrication, as well as various characterisation techniques. Noteworthy, the multiple use of PSNPs in different disciplines such as biomedical, cosmetics agrochemicals, energy storage, water detoxification, and food-related realms, is accounted in detail. Insights into the toxicological impacts of the PSNPs and their possible risks to human health are addressed, and efforts made in terms of PSNPs development and optimising strategies that allow for enhanced delivery are highlighted. Finally, limitations, potential drawbacks, market diffusion, economic viability and future possibilities for PSNPs to achieve widespread commercial use are also discussed.
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Nanopartículas , Polisacáridos , HumanosRESUMEN
Sulfonated lignin can significantly enhance the enzymatic hydrolysis of lignocellulose substrates. Lignin is a type of polyphenol, therefore, sulfonated polyphenol, such as tannic acid, is likely to have similar effects. In order to obtain a low-cost and high-efficiency additive to improve enzymatic hydrolysis, sulfomethylated tannic acids (STAs) with different sulfonation degrees were prepared and their impact on enzymatic saccharification of sodium hydroxide-pretreated wheat straw were investigated. Tannic acid strongly inhibited, while STAs strongly promoted the substrate enzymatic digestibility. While adding 0.04 g/g-substrate STA containing 2.4 mmol/g sulfonate group, the glucose yield increased from 60.6% to 97.9% at a low cellulase dosage (5 FPU/g-glucan). The concentration of protein in enzymatic hydrolysate significantly increased with the added STAs, indicating that cellulase preferentially adsorbed with STAs, thereby reducing the amount of cellulase nonproductively anchored on substrate lignin. This result provides a reliable approach for establishing an efficient lignocellulosic enzyme hydrolysis system.
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Celulasa , Lignina , Lignina/metabolismo , Triticum/metabolismo , Hidróxido de Sodio , Azúcares , Hidrólisis , Celulasa/metabolismo , PolifenolesRESUMEN
Cellulose materials have poor wet strength and are susceptible to acidic or basic environments. Herein, we developed a facile strategy to modify bacterial cellulose (BC) with a genetically engineered Family 3 Carbohydrate-Binding Module (CBM3). To assess the effect of BC films, water adsorption rate (WAR), water holding capacity (WHC), water contact angle (WCA), and mechanical and barrier properties were determined. The results showed that CBM3-modified BC film exhibited significant strength and ductility improvement, reflecting improved mechanical properties of the film. The excellent wet strength (both in the acidic and basic environment), bursting strength, and folding endurance of CBM3-BC films were due to the strong interaction between CBM3 and fiber. The toughness of CBM3-BC films reached 7.9, 28.0, 13.3, and 13.6 MJ/m3, which were 6.1, 1.3, 1.4, and 3.0 folds over the control for conditions of dry, wet, acidic, and basic, respectively. In addition, its gas permeability was reduced by 74.3 %, and folding times increased by 56.8 % compared with the control. The synthesized CBM3-BC films may hold promise for future applications in food packaging, paper straw, battery separator, and other fields. Finally, the in situ modification strategy used to BC can be successfully applied in other functional modifications for BC materials.
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Celulosa , Agua , Celulosa/química , Agua/química , Resistencia a la TracciónRESUMEN
Cationic starch is the most widely used paper strength additive for papermaking wet end applications. However, it remains unclear how differently quaternized amylose (QAM) and amylopectin (QAP) are adsorbed on the fiber surface and their relative contribution to the inter-fiber bonding of papers. Herein, separated amylose and amylopectin were quaternized with different degrees of substitution (DS). After that, the adsorption behaviors of QAM and QAP on the fiber surface, the viscoelastic properties of the adlayers and their strength enhancement to fiber networks were comparatively characterized. Based on the results, the morphology visualizations of the starch structure displayed a strong impact on the adsorbed structural distributions of QAM and QAP. QAM adlayer with a helical linear or slightly branched structure was thin and rigid, while the QAP adlayer with a highly branched structure was thick and soft. In addition, the DS, pH and ionic strength had some impacts on the adsorption layer as well. Regarding the paper strength enhancement, the DS of QAM correlated positively to the paper strength, whereas the DS of QAP correlated inversely. The results provide a deep understanding of the impacts of starch morphology on performance and offer us some practical guidelines in starch selection.
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Amilopectina , Amilosa , Amilopectina/química , Amilosa/química , Adsorción , Almidón/química , CarbohidratosRESUMEN
As a natural green polymer, chitosan is a promising material for plastic replacement. However, the mutually exclusive strength and toughness severely limit its commercial application, and the improved strength of chitosan-based materials is typically achieved at the expense of elongation or toughness. Herein, inspired by the existed multiple non-covalent interactions in biosynthesized fibers, we successfully fabricated a high-performance lignin/chitosan composite film by constructing sacrificial conjoined-network (hydrogen bonds, electrostatic interaction, etc.), which results in an impressive enhancement in tensile strength (50.2 MPa), elongation (73.6 %), and toughness (2.7 MJ/m3) simultaneously, much superior to the pure chitosan film. In addition, the composite film also demonstrates excellent UV resistance, thermal stability, low oxygen permeability (3.9 cm3/(m2·24hâ§0.1 MPa)) and food preservation (with no negligible change for grape, apple, and cherry tomato after 5-10 days). Such developed lignin/chitosan with both components from biomass represents a promising alternative for plastic replacement.
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Quitosano , Quitosano/química , Lignina , Resistencia a la Tracción , Plásticos , Conservación de AlimentosRESUMEN
The combination of optical transparency and mechanical strength is a highly desirable attribute of wood-based glazing materials. However, such properties are typically obtained by impregnation of the highly anisotropic wood with index-matching fossil-based polymers. In addition, the presence of hydrophilic cellulose leads to a limited water resistance. Herein, this work reports on an adhesive-free lamination that uses oxidation and densification to produce transparent all-biobased glazes. The latter are produced from multilayered structures, free of adhesives or filling polymers, simultaneously displaying high optical clarity and mechanical strength, in both dry and wet conditions. Specifically, high values of optical transmittance (≈85.4%), clarity (≈20% with low haze) at a thickness of ≈0.3 mm, and highly isotropic mechanical strength and water resistance (wet strength of ≈128.25 MPa) are obtained for insulative glazes exhibiting low thermal conductivity (0.27 W m-1 K-1 , almost four times lower than glass). The proposed strategy results in materials that are systematically tested, with the leading effects of self-adhesion induced by oxidation rationalized by ab initio molecular dynamics simulation. Overall, this work demonstrates wood-derived materials as promising solutions for energy-efficient and sustainable glazing applications.
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We introduce a strategy to disintegrate cellulose microfibrils present in the cell walls of plant fibers. The process includes impregnation and mild oxidation followed by ultrasonication, which loosens the hydrophilic planes of crystalline cellulose while preserving the hydrophobic ones. The resultant molecularly-sized cellulose structures (cellulose ribbons, CR) retain a length of the order of a micron (1.47 ± 0.48 µm, AFM). A very high axial aspect ratio is determined (at least 190), considering the CR height (0.62 ± 0.38 nm, AFM), corresponding to 1-2 cellulose chains, and width (7.64 ± 1.82 nm, TEM). The new molecularly-thin cellulose proposes excellent hydrophilicity and flexibility, enabling a remarkable viscosifying effect when dispersed in aqueous media (shear-thinning, zero shear viscosity of 6.3 × 105 mPa·s). As such, CR suspensions readily develop into gel-like Pickering emulsions in the absence of crosslinking, suitable for direct ink writing at ultra-low solids content.
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Lignin, as a precious resource given to mankind by nature with abundant functional aromatic structures, has drawn much attention in the recent decade from academia to industry worldwide, aiming at harvesting aromatic compounds from this abundant and renewable natural polymer resource. How to efficiently depolymerize lignin to easy-to-handle aromatic monomers is the precondition of lignin utilization. Many strategies/methods have been developed to effectively degrade lignin into monomers, such as the traditional methods of pyrolysis, gasification, liquid-phase reforming, solvolysis, chemical oxidation, hydrogenation, reduction, acidolysis, alkaline hydrolysis, alcoholysis, as well as the newly developed redox-neutral process, biocatalysis, and combinatorial strategies. Therefore, there is a strong demand to systemically summarize these developed strategies and methods and reveal the internal transformation principles of the lignin. Focusing on the topic of lignin depolymerization to aromatic chemicals, this review reorganizes and categorizes the strategies/methods according to their mechanisms, orbiting the center of critical intermediates during the lignin linkage transformation, which includes the critical anionic intermediates, cationic intermediates, organometallic intermediates, organic molecular intermediates, aryl cation radical intermediates, and neutral radical intermediates. The corresponding introduction involves the generation and the transformation chemistry of the critical intermediates via the corresponding C-H/O-H/C-C/C-O chemical bond transformations, leading to the cleavage of the C-C/C-O linkage bonds. Accompanying the brief introduction of lignin chemistry and the final concluding remarks and perspectives on lignin depolymerization, this review aims to provide a current research process of lignin depolymerization, which may provide useful suggestions for this vigorous research field.
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Acid pretreatment of biomass decomposed hemicelluloses but could not effectively remove lignin, which hindered biomass saccharification and carbohydrates utilization. In this work, 2-naphthol-7-sulfonate (NS) and sodium bisulfite (SUL) were simultaneously added to acid pretreatment, which was found to synergistically increase hydrolysis yield of cellulose from 47.9 % to 90.6 %. Based on in-depth investigations, strong linear correlations were observed between cellulose accessibility and lignin removal, fiber swelling, CrI/cellulose ratio, cellulose crystallite size, respectively, indicating that some physicochemical characteristics of cellulose played significant roles in improving cellulose hydrolysis yield. After enzymatic hydrolysis, 84 % carbohydrates could be liberated and recovered as fermentable sugars for subsequent utilization. Mass balance illustrated that for 100 kg raw biomass, 15.1 kg xylonic acid and 20.5 kg ethanol could be co-produced, indicating the efficient utilization of biomass carbohydrates.