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From, M., Larsson, P. T., Andreasson, B., Medronho, B., Svanedal, I., Edlund, H. & Norgren, M. (2020). Tuning the properties of regenerated cellulose: Effects of polarity and water solubility of the coagulation medium. Carbohydrate Polymers, 236, Article ID 116068.
Open this publication in new window or tab >>Tuning the properties of regenerated cellulose: Effects of polarity and water solubility of the coagulation medium
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2020 (English)In: Carbohydrate Polymers, ISSN 0144-8617, E-ISSN 1879-1344, Vol. 236, article id 116068Article in journal (Refereed) Published
Abstract [en]

In this study, the effect of different alcohols and esters as a coagulation medium in the regeneration of cellulose dissolved in an aqueous LiOH-urea-based solvent was thoroughly investigated using various methods such as solid state NMR, X-ray diffraction, water contact angle, oxygen gas permeability, mechanical testing, and scanning electron microscopy. It was observed that several material properties of the regenerated cellulose films follow trends that correlate to the degree of cellulose II crystallinity, which is determined to be set by the miscibility of the coagulant medium (nonsolvent) and the aqueous alkali cellulose solvent rather than the nonsolvents’ polarity. This article provides an insight, thus creating a possibility to carefully tune and control the cellulose material properties when tailor-made for different applications. 

Keywords
Cellulose, Coagulation medium, Crystallinity, Polarity, Regeneration
National Category
Chemical Sciences
Identifiers
urn:nbn:se:miun:diva-38656 (URN)10.1016/j.carbpol.2020.116068 (DOI)000519306900074 ()2-s2.0-85080088394 (Scopus ID)
Available from: 2020-03-16 Created: 2020-03-16 Last updated: 2020-04-03Bibliographically approved
Yang, J., Zasadowski, D., Edlund, H. & Norgren, M. (2019). Biorefining of Spruce TMP Process Water: Selective Fractionation of Lipophilic Extractives with Induced Air Flotation and Surface Active Additive. BioResources, 14(2), 4124-4135
Open this publication in new window or tab >>Biorefining of Spruce TMP Process Water: Selective Fractionation of Lipophilic Extractives with Induced Air Flotation and Surface Active Additive
2019 (English)In: BioResources, ISSN 1930-2126, E-ISSN 1930-2126, Vol. 14, no 2, p. 4124-4135Article in journal (Refereed) Published
Abstract [en]

Lignocellulose biomass plays an important role in reducing thedependency on fossil fuels and ameliorating the dire consequences ofclimate change. It is therefore important that all the components oflignocellulose biomass are exploited. These components includehemicelluloses and extractives that are liberated and sterically stabilizedduring the thermomechanical pulping and that form the dissolved andcolloidal substance (DCS) in the process water. Biorefining of this processwater can extract these substances, which have a number of promisingapplications and can contribute to the full exploitation of lignocellulosebiomass. This paper presents a simple treatment of unbleached Norwayspruce (Picea abies) process water from TMP (thermomechanical pulping)production using induced air flotation (IAF) and cationic surfactant,dodecyl trimethylammonium chloride (DoTAC) to refine the extractivesand prepare the waters so that hemicellulose could be easily harvested ata later stage. By applying 80 ppm of DoTAC at a pH of 3.5 and 50 °Cbefore induced air flotation, 94% of the lipophilic extractives wererecovered from process water. Dissolved hemicellulose polysaccharideswere cleansed and left in the treated process water. The process enabledefficient biorefining of lipophilic extractives and purification of the processwater to enable more selective harvesting of hemicelluloses in subsequentsteps.

Keywords
Biorefining; Lipophilic extractives; Thermomechanical pulping; Induced air flotation
National Category
Chemical Engineering
Identifiers
urn:nbn:se:miun:diva-35955 (URN)10.15376/biores.14.2.4124-4135 (DOI)000466449000115 ()2-s2.0-85071077339 (Scopus ID)
Projects
EU Reginal fund 2
Funder
European Regional Development Fund (ERDF)
Available from: 2019-04-05 Created: 2019-04-05 Last updated: 2019-09-03Bibliographically approved
Costa, C., Medronho, B., Filipe, A., Mira, I., Lindman, B., Edlund, H. & Norgren, M. (2019). Emulsion formation and stabilization by biomolecules: The leading role of cellulose. Polymers, 11(10), Article ID 1570.
Open this publication in new window or tab >>Emulsion formation and stabilization by biomolecules: The leading role of cellulose
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2019 (English)In: Polymers, ISSN 2073-4360, E-ISSN 2073-4360, Vol. 11, no 10, article id 1570Article in journal (Refereed) Published
Abstract [en]

Emulsion stabilization by native cellulose has been mainly hampered because of its insolubility in water. Chemical modification is normally needed to obtain water-soluble cellulose derivatives. These modified celluloses have been widely used for a range of applications by the food, cosmetic, pharmaceutic, paint and construction industries. In most cases, the modified celluloses are used as rheology modifiers (thickeners) or as emulsifying agents. In the last decade, the structural features of cellulose have been revisited, with particular focus on its structural anisotropy (amphiphilicity) and the molecular interactions leading to its resistance to dissolution. The amphiphilic behavior of native cellulose is evidenced by its capacity to adsorb at the interface between oil and aqueous solvent solutions, thus being capable of stabilizing emulsions. In this overview, the fundamentals of emulsion formation and stabilization by biomolecules are briefly revisited before different aspects around the emerging role of cellulose as emulsion stabilizer are addressed in detail. Particular focus is given to systems stabilized by native cellulose, either molecularly-dissolved or not (Pickering-like effect). 

Keywords
Adsorption, Amphiphilicity, Cellulose, Emulsion stability, Oil-water interface
National Category
Chemical Engineering
Identifiers
urn:nbn:se:miun:diva-37680 (URN)10.3390/polym11101570 (DOI)000495382700039 ()31561633 (PubMedID)2-s2.0-85073478887 (Scopus ID)
Available from: 2019-11-14 Created: 2019-11-14 Last updated: 2020-01-15Bibliographically approved
From, M., Andreasson, B., Svanedal, I., Larsson, T., Edlund, H. & Norgren, M. (2019). Influence of regeneration liquid polarity on different material properties of dried cellulose II films. Abstracts of Papers of the American Chemical Society, 257, Article ID 120.
Open this publication in new window or tab >>Influence of regeneration liquid polarity on different material properties of dried cellulose II films
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2019 (English)In: Abstracts of Papers of the American Chemical Society, ISSN 0065-7727, Vol. 257, article id 120Article in journal, Meeting abstract (Refereed) Published
National Category
Chemical Engineering
Identifiers
urn:nbn:se:miun:diva-38459 (URN)000478860502524 ()
Note

National Meeting of the American-Chemical-Society (ACS), Orlando, FL, MAR 31-APR 04, 2019

Available from: 2020-02-19 Created: 2020-02-19 Last updated: 2020-02-19Bibliographically approved
Costa, C., Mira, I., Benjamins, J.-W., Lindman, B., Edlund, H. & Norgren, M. (2019). Interfacial activity and emulsion stabilization of dissolved cellulose. Journal of Molecular Liquids, 292, Article ID 111325.
Open this publication in new window or tab >>Interfacial activity and emulsion stabilization of dissolved cellulose
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2019 (English)In: Journal of Molecular Liquids, ISSN 0167-7322, E-ISSN 1873-3166, Vol. 292, article id 111325Article in journal (Refereed) Published
Abstract [en]

Some aspects of the interfacial behavior of cellulose dissolved in an aqueous solvent were investigated. Cellulose was found to significantly decrease the interfacial tension (IFT) between paraffin oil and 85 wt% phosphoric acid aqueous solutions. This decrease was similar in magnitude to that displayed by non-ionic cellulose derivatives. Cellulose's interfacial activity indicated a significant amphiphilic character and that the interfacial activity of cellulose derivatives is not only related to the derivatization but inherent in the cellulose backbone. This finding suggests that cellulose would have the ability of stabilizing dispersions, like oil-in-water emulsions in a similar way as a large number of cellulose derivatives. In its molecularly dissolved state, cellulose proved to be able to stabilize emulsions of paraffin in the polar solvent on a short-term. However, long-term stability against drop-coalescence was possible to achieve by a slight change in the amphiphilicity of cellulose, effected by a slight increase in pH. These emulsions exhibited excellent stability against coalescence/oiling-off over a period of one year. Ageing of the cellulose solution before emulsification (resulting in molecular weight reduction) was found to favour the creation of smaller droplets. 

Keywords
Adsorption, Amphiphilicity, Cellulose molecules, Emulsions, Interfacial activity, Oil-water interface
National Category
Chemical Engineering
Identifiers
urn:nbn:se:miun:diva-36838 (URN)10.1016/j.molliq.2019.111325 (DOI)000488658900015 ()2-s2.0-85069688256 (Scopus ID)
Note

Available under a Creative Commons license https://creativecommons.org/licenses/by/4.0/

Available from: 2019-08-13 Created: 2019-08-13 Last updated: 2019-11-13Bibliographically approved
Eivazihollagh, A., Svanedal, I., Edlund, H. & Norgren, M. (2019). On chelating surfactants: Molecular perspectives and application prospects. Journal of Molecular Liquids, 278, 688-705
Open this publication in new window or tab >>On chelating surfactants: Molecular perspectives and application prospects
2019 (English)In: Journal of Molecular Liquids, ISSN 0167-7322, E-ISSN 1873-3166, Vol. 278, p. 688-705Article in journal, Editorial material (Refereed) Published
Abstract [en]

Chelating agents, molecules that very strongly coordinates certain metal ions, are used industrially as well as in consumer products to minimize disturbances and increase performance of reactions and applications. The widely used sequestering agents, nitrilotriacetic acid (NTA), ethylenediaminetetraacetic acid (EDTA) and diethylenetriaminepentaacetic acid (DTPA) belong to this branch of readily water-soluble compounds. When these chemical structures also have hydrophobic parts, they are prone to adsorb at air-water interfaces and to self-assemble. Such bifunctional molecules can be called chelating surfactants and will have more extended utilization prospects than common chelating agents or ordinary ionic surfactants. The present review attempts to highlight the fundamental behavior of chelating surfactants in solution and at interfaces, and their very specific interactions with metal ions. Methods to recover chelating surfactants from metal chelates are also described. Moreover, utilization of chelating surfactants in applications for metal removal in environmental engineering and mineral processing, as well as for metal control in the fields of biology, chemistry and physics, is exemplified and discussed.

Keywords
Chelating surfactants, Metallosurfactants, Amphiphiles, Self-assembly, Metal-coordination, Sequestering agents, Complexing agents, Remediation, Flotation, Metal recovery, Recovery, Catalysis, Metalloenzymes, Contrast agents, Nanoparticle synthesis, Applications
National Category
Mineral and Mine Engineering Nano Technology Bioremediation Water Treatment Environmental Management Paper, Pulp and Fiber Technology Bio Materials Biocatalysis and Enzyme Technology Chemical Engineering Other Chemical Engineering Other Engineering and Technologies not elsewhere specified
Identifiers
urn:nbn:se:miun:diva-35610 (URN)10.1016/j.molliq.2019.01.076 (DOI)000461526600074 ()2-s2.0-85061119211 (Scopus ID)
Available from: 2019-02-08 Created: 2019-02-08 Last updated: 2019-05-20Bibliographically approved
Yang, J., Dahlström, C., Edlund, H., Lindman, B. & Norgren, M. (2019). pH-responsive cellulose–chitosan nanocomposite films with slow release of chitosan. Cellulose (London), 26(6), 3763-3776
Open this publication in new window or tab >>pH-responsive cellulose–chitosan nanocomposite films with slow release of chitosan
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2019 (English)In: Cellulose (London), ISSN 0969-0239, E-ISSN 1572-882X, Vol. 26, no 6, p. 3763-3776Article in journal (Refereed) Published
Abstract [en]

Cellulose–chitosan films were preparedusing a physical method in which cellulose andchitosan were separately dissolved via freeze thawingin LiOH/urea and mixed in different proportions, theresulting films being cast and regenerated in water/ethanol. X-ray diffraction and Fourier transforminfrared spectroscopy (FT-IR) spectroscopy verifiedthe composition changes in the nanocomposites due todifferent mixing ratios between the polymers. Tensilestress–strain measurements indicated that the mechan-ical performance of the cellulose–chitosan nanocom-posites slightly worsened with increasing chitosancontent compared with that of films comprisingcellulose alone. Field emission scanning electronmicroscopy revealed the spontaneous formation ofnanofibers in the films; these nanofibers were subse-quently ordered into lamellar structures. Water uptakeand microscopy analysis of film thickness changesindicated that the swelling dramatically increased atlower pH and with increasing chitosan content, thisbeing ascribed to the Gibbs–Donnan effect. Slowmaterial loss appeared at acidic pH, as indicated by aloss of weight, and quantitative FT-IR analysisconfirmed that chitosan was the main componentreleased.Asample containing 75% chitosan reached amaximum swelling ratio and weight loss of 1500%and 55 wt%, respectively, after 12 h at pH 3. Thestudy presents a novel way of preparing pH-responsivecellulose–chitosan nanocomposites with slow-releasecharacteristics using an environmentally friendlyprocedure and without any chemical reactions.

Keywords
Cellulose dissolution, Chitosan dissolution, pH responsive, Gibbs–Donnan equilibrium, Nanocomposite, Slow release
National Category
Other Chemical Engineering
Identifiers
urn:nbn:se:miun:diva-35778 (URN)10.1007/s10570-019-02357-5 (DOI)000464849500011 ()2-s2.0-85062686323 (Scopus ID)
Funder
Swedish Research Council Formas, 942-2015-251
Available from: 2019-03-12 Created: 2019-03-12 Last updated: 2019-09-03Bibliographically approved
Eivazihollagh, A., Löf, L., Lindman, B., Norgren, M. & Edlund, H. (2019). Vesicle-templated all-cellulose nanocapsules. In: : . Paper presented at 6th EPNOE International Polysaccharide Conference, Aveiro, Portugal, 21–25 October, 2019.
Open this publication in new window or tab >>Vesicle-templated all-cellulose nanocapsules
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2019 (English)Conference paper, Poster (with or without abstract) (Refereed)
Abstract [en]

Polymeric multilayers capsules constructed using the layer-by-layer (LbL) technique are interesting candidates for the purposes of storage, encapsulation and release in a wide range of biomedical applications. In the current study, cellulose-based nanocapsules were produced via the LbL technique. In this procedure, alternating deposition of the two biocompatible polymers anionic cellulose, carboxymethylcellulose (CMC), and cationic cellulose, quaternized hydroxyethylcellulose ethoxylate (QHECE), on a cationic vesicular template made of didodecyldimethylammonium bromide (DDAB), was performed. The obtained nanocapsules, were characterized by dynamic light scattering (DLS), ⇣ potential measurements, and field-emission scanning electron microscopy (FE-SEM). DLS measurements revealed that the size of the spheres is about hundreds of nanometer with polydispersity index (PDI) values between 0.2 and 0.3, indicating a relatively homogeneous size distribution. In addition, FESEM characterization also indicated the shape and size of obtained material. The surface charge analysis of the nanocapsules by ⇣ potential measurements indicated the presence of electrostatically stabilized nanoparticles. The values of diameter, PDI and surface charge for cationic vesicles coated by CMC were 204 nm, 0.26 and –38 mV, respectively. After deposition of QHECE, the diameter, PDI, and surface charge were about 265 nm, 0.36 and +32.5 mV, respectively. Figure 1 shows FE-SEM images of cellulose nanoparticles fabricated via LbL deposition of polyelectrolyte layers. As seen in the microscopy images, the shape of the core-shell particles are not fully spherical which could be due to drying e↵ects of the sample before FE-SEM characterization. The construction of cellulose nanocontainers by using an alternating deposition of oppositely charged biobased polyelectrolytes on vesicles o↵ers several advantages such as simplicity, reproducibility, biocompatibility, low-cost, mild reaction conditions, and high controllability over the thickness and composition of the shell.

National Category
Physical Chemistry
Identifiers
urn:nbn:se:miun:diva-37815 (URN)
Conference
6th EPNOE International Polysaccharide Conference, Aveiro, Portugal, 21–25 October, 2019
Funder
ÅForsk (Ångpanneföreningen's Foundation for Research and Development)
Available from: 2019-11-28 Created: 2019-11-28 Last updated: 2019-12-09Bibliographically approved
Eivazihollagh, A., Norgren, M., Dahlström, C. & Edlund, H. (2018). Controlled Synthesis of Cu and Cu2O NPs and Incorporation of Octahedral Cu2O NPs in Cellulose II Films. Nanomaterials, 8(4), Article ID 238.
Open this publication in new window or tab >>Controlled Synthesis of Cu and Cu2O NPs and Incorporation of Octahedral Cu2O NPs in Cellulose II Films
2018 (English)In: Nanomaterials, ISSN 2079-4991, Vol. 8, no 4, article id 238Article in journal (Refereed) Published
Abstract [en]

In this study, Cu and Cu2O nanoparticles (NPs) were synthesized through chemical reduction of soluble copper-chelating ligand complexes using formaldehyde as a reducing agent. The influence of various chelating ligands, such as ethylenediaminetetraacetic acid (EDTA), diethylenetriaminepentaacetic acid (DTPA), and a surface-active derivative of DTPA (C12-DTPA), as well as surfactants (i.e., hexadecyltrimethylammonium bromide (CTAB), dodecyltrimethylammonium chloride (DoTAC), sodium dodecyl sulfate (SDS), and dimethyldodecylamine-N-oxide (DDAO)), on morphology and the composition of produced NPs was investigated. In the absence of surfactants, spherical copper particles with polycrystalline structure could be obtained. X-ray diffraction (XRD) analysis revealed that, in the presence of EDTA, the synthesized NPs are mainly composed of Cu with a crystallite size on the order of 35 nm, while with DTPA and C12-DTPA, Cu2O is also present in the NPs as a minority phase. The addition of ionic surfactants to the copper–EDTA complex solution before reduction resulted in smaller spherical particles, mainly composed of Cu. However, when DDAO was added, pure Cu2O nano-octahedrons were formed, as verified by high-resolution scanning electron microscopy (HR-SEM) and XRD. Furthermore, a hybrid material could be successfully prepared by mixing the octahedral Cu2O NPs with cellulose dissolved in a LiOH/urea solvent system, followed by spin-coating on silica wafers. It is expected that this simple and scalable route to prepare hybrid materials could be applied to a variety of possible applications.

Keywords
copper nanoparticles; cuprous oxide nano-octahedrons; hybrid material; regenerated cellulose; chemical reduction; chelating agent; surfactant
National Category
Nano Technology Chemical Engineering Materials Engineering
Identifiers
urn:nbn:se:miun:diva-33497 (URN)10.3390/nano8040238 (DOI)000434889100059 ()2-s2.0-85045875998 (Scopus ID)
Available from: 2018-04-16 Created: 2018-04-16 Last updated: 2018-07-04Bibliographically approved
Ibrahem, I., Iqbal, M. N., Verho, O., Eivazihollagh, A., Olsén, P., Edlund, H., . . . Johnston, E. V. (2018). Copper Nanoparticles on Controlled Pore Glass and TEMPO for the Aerobic Oxidation of Alcohols. ChemNanoMat, 4(1), 71-75
Open this publication in new window or tab >>Copper Nanoparticles on Controlled Pore Glass and TEMPO for the Aerobic Oxidation of Alcohols
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2018 (English)In: ChemNanoMat, ISSN 2199-692X, Vol. 4, no 1, p. 71-75Article in journal (Refereed) Published
Abstract [en]

Herein, we report on the facile synthesis of a heterogeneous copper nanocatalyst and its combination with 2,2,6,6-tetramethyl-1-piperidinyloxy (TEMPO) for the aerobic oxidation of alcohols to their corresponding carbonyl compounds. This low cost copper nanocatalyst was found to exhibit excellent recyclability, making it a highly attractive catalytic system from an economical and environmental point of view. Extensive characterization of the catalyst by a number of techniques revealed that it was comprised of well-dispersed Cu(I/II) nanoparticles with an average size of around 6nm.

Keywords
Alcohol oxidation, Copper nanoparticles, Green chemistry, Heterogeneous catalysis, TEMPO
National Category
Chemical Sciences
Identifiers
urn:nbn:se:miun:diva-32328 (URN)10.1002/cnma.201700309 (DOI)000419237800011 ()2-s2.0-85033664510 (Scopus ID)
Note

Version of record online: 14 November 2017

Available from: 2017-12-07 Created: 2017-12-07 Last updated: 2019-08-06Bibliographically approved
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Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0002-5579-3373

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