Browsing by Author "Norgren, Magnus"
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- Brief overview on bio-based adhesives and sealantsPublication . Magalhães, Solange; Alves, Luís; Medronho, Bruno; Fonseca, Ana C.; Romano, Anabela; Coelho, Jorge F.J.; Norgren, MagnusAdhesives and sealants (AS) are materials with excellent properties, versatility, and simple curing mechanisms, being widely used in different areas ranging from the construction to the medical sectors. Due to the fast-growing demand for petroleum-based products and the consequent negative environmental impact, there is an increasing need to develop novel and more sustainable sources to obtain raw materials (monomers). This reality is particularly relevant for AS industries, which are generally dependent on non-sustainable fossil raw materials. In this respect, biopolymers, such as cellulose, starch, lignin, or proteins, emerge as important alternatives. Nevertheless, substantial improvements and developments are still required in order to simplify the synthetic routes, as well as to improve the biopolymer stability and performance of these new bio-based AS formulations. This environmentally friendly strategy will hopefully lead to the future partial or even total replacement of non-renewable petroleum-based feedstock. In this brief overview, the general features of typical AS are reviewed and critically discussed regarding their drawbacks and advantages. Moreover, the challenges faced by novel and more ecological alternatives, in particular lignocellulose-based solutions, are highlighted.
- Cellulose-stabilized oil-in-water emulsions: structural features, microrheology, and stabilityPublication . Costa, Carolina; Rosa, Pedro; Filipe, Alexandra; Medronho, Bruno; Romano, Anabela; Liberman, Lucy; Talmon, Yeshayahu; Norgren, MagnusCellulose-based oil-in-water (O/W) emulsions were studied by diffusing wave spectroscopy (DWS) regarding the effect of the cellulose concentration and mixing rate on the average droplet size, microrheological features and stability. Furthermore, the microstructure of these emulsions was imaged by cryo-scanning electron microscopy (cryo-SEM). The micrographs showed that cellulose was effectively adsorbed at the oil-water interface, resembling a film-like shell that protected the oil droplets from coalescing. The non-adsorbed cellulose that was observed in the continuous aqueous medium, contributed to the enhancement of the viscosity of the medium, leading to an improvement in the stability of the overall system. Generally, the higher the cellulose concentration and mixing rate, the smaller the emulsion droplets formed, and the higher was their stability. The combination of both techniques, DWS and cryo-SEM, revealed a very appealing and robust methodology for the characterization and design of novel emulsion-based formulations.
- Engineering novel phenolic foams with lignin extracted from pine wood residues via a new levulinic-acid assisted processPublication . Melro, Elodie; Duarte, Hugo; Antunes, Filipe E.; Valente, Artur J.M.; Romano, Anabela; Norgren, Magnus; Medronho, BrunoPhenolic foams are typically produced from phenolic resins, using phenol and formaldehyde precursors. Therefore, common phenolic foams are non-sustainable, comprising growing environmental, health, and economic concerns. In this work, lignin extracted from pine wood residues using a "green" levulinic acid-based solvent, was used to partially substitute non-sustainable phenol. The novel engineered foams were systematically compared to foams composed of different types of commercially available technical lignins. Different features were analyzed, such as foam density, microstructure (electron microscopy), surface hydrophilicity (contact angle), chemical grafting (infrared spectroscopy) and mechanical and thermal features. Overall, it was observed that up to 30 wt% of phenol can be substituted by the new type of lignin, without compromising the foam properties. This work provides a new insights on the development of novel lignin-based foams as a very promising sustainable and renewable alternative to petrol-based counterparts.
- Hydrophobic interactions control the self-assembly of DNA and cellulosePublication . Lindman, Björn; Medronho, Bruno; Alves, Luís; Norgren, Magnus; Nordenskiöld, LarsDesoxyribosenucleic acid, DNA, and cellulose molecules self-assemble in aqueous systems. This aggregation is the basis of the important functions of these biological macromolecules. Both DNA and cellulose have significant polar and nonpolar parts and there is a delicate balance between hydrophilic and hydrophobic interactions. The hydrophilic interactions related to net charges have been thoroughly studied and are well understood. On the other hand, the detailed roles of hydrogen bonding and hydrophobic interactions have remained controversial. It is found that the contributions of hydrophobic interactions in driving important processes, like the double-helix formation of DNA and the aqueous dissolution of cellulose, are dominating whereas the net contribution from hydrogen bonding is small. In reviewing the roles of different interactions for DNA and cellulose it is useful to compare with the self-assembly features of surfactants, the simplest case of amphiphilic molecules. Pertinent information on the amphiphilic character of cellulose and DNA can be obtained from the association with surfactants, as well as on modifying the hydrophobic interactions by additives.
- Levulinic acid-based “green” solvents for lignocellulose fractionation: on the superior extraction yield and selectivity toward ligninPublication . Melro, Elodie; Riddell, Alexander; Bernin, Diana; Rosa Da Costa, Ana; Valente, Artur J. M.; Antunes, Filipe E.; Romano, Anabela; Norgren, Magnus; Medronho, BrunoThe high potential use of lignin in novel biomaterialsand chemicalsrepresents an important opportunity for the valorization of the mostabundant natural resource of aromatic molecules. From an environmentalperspective, it is highly desirable replacing the hazardous methodscurrently used to extract lignin from lignocellulosic biomass anddevelop more sustainable and environmentally friendly approaches.Therefore, in this work, levulinic acid (a "green" solventobtained from biomass) was successfully used, for the first time,to selectively extract high-quality lignin from pine wood sawdustresidues at 200 degrees C for 6 h (at atmospheric pressure). Moreover,the addition of catalytic concentrations of inorganic acids (i.e.,H2SO4 or HCl) was found to substantially reducethe temperature and reaction times needed (i.e., 140 degrees C, 2 h)for complete lignin extraction without compromising its purity. NMRdata suggests that condensed OH structures and acidic groups are presentin the lignin following extraction. Levulinic acid can be easily recycledand efficiently reused several times without affecting its performance.Furthermore, excellent solvent reusability and performance of extractionof other wood residues has been successfully demonstrated, thus makingthe developed levulinic acid-based procedure highly appealing andpromising to replace the traditional less sustainable methodologies.
- Levulinic acid: a novel sustainable solvent for lignin dissolutionPublication . Melro, Elodie; Filipe, Alexandra; Valente, Artur J. M.; Antunes, Filipe E.; Romano, Anabela; Norgren, Magnus; Medronho, BrunoLignin is a natural, renewable resource with potential to be used in biomaterials. Due to its complex structure, its efficient dissolution is still challenging, which hinders its applicability at large scale. This challenge become harder considering the current need of sustainable and environmentally friendly solvents. To the best of our knowledge, this work reports for the first time the dissolution of kraft lignin in levulinic acid, a "green" solvent, and compares its efficiency with common carboxylic acids and sulfuric acid. It has been found that levulinic acid has a high capacity to dissolve kraft lignin at room temperature (40 wt% solubility), and it efficiency is not compromised when diluting the acid with water (up to 40 wt% water content). the Kamlet-Taft pi* parameter of the different acidic solvents was estimated and found to correlate well with their solubility performance. Lignins previously dissolved in levulinic and formic acids were selected to be regenerated and minor differences were found in thermal stability and morphological structure, when compared to native kraft lignin. However, an increase in the content of the carbonyl groups in the regenerated lignin material was observed. (C) 2020 Elsevier B.V. All rights reserved.
- Lignin enhances cellulose dissolution in cold alkaliPublication . Costa, Carolina; Medronho, Bruno; Eivazi, Alireza; Svanedal, Ida; Lindman, Björn; Edlund, Håkan; Norgren, MagnusAqueous sodium hydroxide solutions are extensively used as solvents for lignin in kraft pulping. These are also appealing systems for cellulose dissolution due to their inexpensiveness, ease to recycle and low toxicity. Cellulose dissolution occurs in a narrow concentration region and at low temperatures. Dissolution is often incomplete but additives, such as zinc oxide or urea, have been found to significantly improve cellulose dissolution. In this work, lignin was explored as a possible beneficial additive for cellulose dissolution. Lignin was found to improve cellulose dissolution in cold alkali, extending the NaOH concentration range to lower values. The regenerated cellulose material from the NaOH-lignin solvents was found to have a lower crystallinity and crystallite size than the samples prepared in the neat NaOH and NaOH-urea solvents. Beneficial lignin-cellulose interactions in solution state appear to be preserved under coagulation and regeneration, reducing the tendency of crystallization of cellulose.
- Lignin-furanic rigid foams: Enhanced methylene blue removal capacity, recyclability, and flame retardancyPublication . Duarte, Hugo; Brás, João; Saoudi Hassani, El Mokhtar; Aliaño González, María José; Magalhães, Solange; Alves, Luís; Valente, Artur J. M.; Eivazi, Alireza; Norgren, Magnus; Romano, Anabela; Medronho, BrunoWorldwide, populations face issues related to water and energy consumption. Water scarcity has intensified globally, particularly in arid and semiarid regions. Projections indicate that by 2030, global water demand will rise by 50%, leading to critical shortages, further intensified by the impacts of climate change. Moreover, wastewater treatment needs further development, given the presence of persistent organic pollutants, such as dyes and pharmaceuticals. In addition, the continuous increase in energy demand and rising prices directly impact households and businesses, highlighting the importance of energy savings through effective building insulation. In this regard, tannin-furanic foams are recognized as promising sustainable foams due to their fire resistance, low thermal conductivity, and high water and chemical stability. In this study, tannin and lignin rigid foams were explored not only for their traditional applications but also as versatile materials suitable for wastewater treatment. Furthermore, a systematic approach demonstrates the complete replacement of the tannin-furan foam phenol source with two lignins that mainly differ in molecular weight and pH, as well as how these parameters affect the rigid foam structure and methylene blue (MB) removal capacity. Alkali-lignin-based foams exhibited notable MB adsorption capacity (220 mg g−1), with kinetic and equilibrium data analysis suggesting a multilayer adsorption process. The prepared foams demonstrated the ability to be recycled for at least five adsorption-desorption cycles and exhibited effective flame retardant properties. When exposed to a butane flame for 5 min, the foams did not release smoke or ignite, nor did they contribute to flame propagation, with the red glow dissipating only 20 s after flame exposure.
- On the development of all-cellulose capsules by vesicle-templated Layer-by-Layer assemblyPublication . Eivazi, Alireza; Medronho, Bruno; Lindman, Björn; Norgren, MagnusPolymeric multilayer capsules formed by the Layer-by-Layer (LbL) technique are interesting candidates for the purposes of storage, encapsulation, and release of drugs and biomolecules for pharmaceutical and biomedical applications. In the current study, cellulose-based core-shell particles were developed via the LbL technique alternating two cellulose derivatives, anionic carboxymethylcellulose (CMC), and cationic quaternized hydroxyethylcellulose ethoxylate (QHECE), onto a cationic vesicular template made of didodecyldimethylammonium bromide (DDAB). The obtained capsules were characterized by dynamic light scattering (DLS), ζ potential measurements, and high-resolution scanning electron microscopy (HR-SEM). DLS measurements reveal that the size of the particles can be tuned from a hundred nanometers with a low polydispersity index (deposition of 2 layers) up to micrometer scale (deposition of 6 layers). Upon the deposition of each cellulose derivative, the particle charge is reversed, and pH is observed to considerably affect the process thus demonstrating the electrostatic driving force for LbL deposition. The HR-SEM characterization suggests that the shape of the core-shell particles formed is reminiscent of the spherical vesicle template. The development of biobased nano- and micro-containers by the alternating deposition of oppositely charged cellulose derivatives onto a vesicle template offers several advantages, such as simplicity, reproducibility, biocompatibility, low-cost, mild reaction conditions, and high controllability over particle size and composition of the shell.
- On the formation and stability of cellulose-based emulsions in alkaline systems: effect of the solvent qualityPublication . Costa, Carolina; Medronho, Bruno; Filipe, Alexandra; Romano, Anabela; Lindman, Björn; Edlund, Håkan; Norgren, MagnusWith amphiphilic properties, cellulose molecules are expected to adsorb at the O/W interface and be capable of stabilizing emulsions. The effect of solvent quality on the formation and stability of cellulose-based O/W emulsions was evaluated in different alkaline systems: NaOH, NaOH-urea and tetrabutylammonium hydroxide (TBAH). The optimal solvency conditions for cellulose adsorption at the O/W interface were found for the alkaline solvent with an intermediate polarity (NaOH-urea), which is in line with the favorable conditions for adsorption of an amphiphilic polymer. A very good solvency (in TBAH) and the interfacial activity of the cation lead to lack of stability because of low cellulose adsorption. However, to achieve long-term stability and prevent oil separation in NaOH-urea systems, further reduction in cellulose's solvency was needed, which was achieved by a change in the pH of the emulsions, inducing the regeneration of cellulose at the surface of the oil droplets (in-situ regeneration).