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Publications (10 of 97) Show all publications
Träger, A., Klein, G., Carrick, C., Pettersson, T., Johansson, M., Wågberg, L., . . . Carlmark, A. (2019). Macroscopic cellulose probes for the measurement of polymer grafted surfaces. Cellulose (London), 26(3), 1467-1477
Open this publication in new window or tab >>Macroscopic cellulose probes for the measurement of polymer grafted surfaces
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2019 (English)In: Cellulose (London), ISSN 0969-0239, E-ISSN 1572-882X, Vol. 26, no 3, p. 1467-1477Article in journal (Refereed) Published
Abstract [en]

A synthesis protocol was identified to produce covalent grafting of poly(dimethyl siloxane) from cellulose, based on prior studies of analogous ring opening polymerizations. Following this polymer modification of cellulose, the contact adhesion was anticipated to be modified and varied as a function of the polymer molecular mass. The synthetic details were optimized for a filter paper surface before grafting the polymer from bulk cellulose spheres. The adhesion of the unmodified and grafted, bulk cellulose spheres were evaluated using the Johnson-Kendall-Roberts (JKR) theory with a custom build contact adhesion testing setup. We report the first example of grafting poly(dimethyl siloxane) directly from bulk cellulose using ring opening polymerization. For short grafting lengths, both the JKR work of adhesion and the adhesion energy at the critical energy release rate (G(c)) were comparable to unmodified cellulose beads. When polymer grafting lengths were extended sufficiently where chain entanglements occur, both the JKR work of adhesion and G(c) were increased by as much as 190%. Given the multitude of options available to graft polymers from cellulose, this study shows the potential to use this type of cellulose spheres to study the interaction between different polymer surfaces in a controlled manner. [GRAPHICS] .

Place, publisher, year, edition, pages
SPRINGER, 2019
Keywords
Grafted polymer, Cellulose, Contact mechanics, Adhesion, Johnson-Kendall-Roberts theory
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-247840 (URN)10.1007/s10570-018-2196-2 (DOI)000460617900004 ()
Note

QC 20190326

Available from: 2019-03-26 Created: 2019-03-26 Last updated: 2019-10-29Bibliographically approved
Engström, J., Benselfelt, T., Wågberg, L., D'Agosto, F., Lansalot, M., Carlmark, A. & Malmström, E. (2019). Tailoring adhesion of anionic surfaces using cationic PISA-latexes – towards tough nanocellulose materials in the wet state. Nanoscale, 11, 4287-4302
Open this publication in new window or tab >>Tailoring adhesion of anionic surfaces using cationic PISA-latexes – towards tough nanocellulose materials in the wet state
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2019 (English)In: Nanoscale, ISSN 2040-3364, E-ISSN 2040-3372, Vol. 11, p. 4287-4302Article in journal (Refereed) Published
Abstract [en]

Cationic latexes with Tgs ranging between −40 °C and 120 °C were synthesised using n-butyl acrylate (BA) and/or methyl methacrylate (MMA) as the core polymers. Reversible addition–fragmentation chain transfer (RAFT) combined with polymerisation-induced self-assembly (PISA) allowed for in situ chain-extension of a cationic macromolecular RAFT agent (macroRAFT) of poly(N-[3-(dimethylamino)propyl] methacrylamide) (PDMAPMA), used as stabiliser in so-called surfactant-free emulsion polymerisation. The resulting narrowly distributed nanosized latexes adsorbed readily onto silica surfaces and to model surfaces of cellulose nanofibrils, as demonstrated by quartz crystal microbalance with dissipation monitoring (QCM-D) measurements. Adsorption to anionic surfaces increased when increasing ionic strength to 10 mM, indicating the influence of the polyelectrolyte effect exerted by the corona. The polyelectrolyte corona affected the interactions in the wet state, the stability of the latex and re-dispersibility after drying. The QCM-D measurements showed that a lower Tg of the core results in a more strongly interacting adsorbed layer at the solid–liquid interface, despite a comparable adsorbed mass, indicating structural differences of the investigated latexes in the wet state. The two latexes with Tg below room temperature (i.e. PBATg-40 and P(BA-co-MMA)Tg3) exhibited film formation in the wet state, as shown by AFM colloidal probe measurements. It was observed that P(BA-co-MMA)Tg3 latex resulted in the largest pull-off force, above 200 m Nm−1 after 120 s in contact. The strongest wet adhesion was achieved with PDMAPMA-stabilized latexes soft enough to allow for interparticle diffusion of polymer chains, and stiff enough to create a strong adhesive joint. Fundamental understanding of interfacial properties of latexes and cellulose enables controlled and predictive strategies to produce strong and tough materials with high nanocellulose content, both in the wet and dry state.

National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-241447 (URN)10.1039/C8NR08057G (DOI)000465410200012 ()2-s2.0-85062644682 (Scopus ID)
Note

QC 20190123

Available from: 2019-01-22 Created: 2019-01-22 Last updated: 2019-05-29Bibliographically approved
Gicquel, E., Martin, C., Gauthier, Q., Engström, J., Abbattista, C., Carlmark, A., . . . Bras, J. (2019). Tailoring Rheological Properties of Thermoresponsive Hydrogels through Block Copolymer Adsorption to Cellulose Nanocrystals. Biomacromolecules, 20(7), 2545-2556
Open this publication in new window or tab >>Tailoring Rheological Properties of Thermoresponsive Hydrogels through Block Copolymer Adsorption to Cellulose Nanocrystals
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2019 (English)In: Biomacromolecules, ISSN 1525-7797, E-ISSN 1526-4602, Vol. 20, no 7, p. 2545-2556Article in journal (Refereed) Published
Abstract [en]

This study investigates the adsorption of a block copolymer composed of a poly(2-(dimethylamino)ethyl methacrylate) (PDMAEMA) cationic polyelectrolyte and a poly(di(ethylene glycol) methyl ethermethacrylate) (PDEGMA) on oxidized cellulose nanocrystals (TO-CNCs) to produce hydrogels. PDMEAMA-b-PDEGMA was synthesized by atom-transfer radical polymerization. The extent and dynamics of the adsorption of PDMAEMA-b-PDEGMA on TO-CNCs were determined by electromechanical microbalance and optical techniques. Electrostatic adsorption was identified on TO-CNCs with the quaternized block copolymer. Small-angle neutron scattering experiments were performed to investigate the polymer behavior on the TO-CNC surfaces. Depending on the temperature, block copolymer induces the aggregation of nanocrystals after adsorption by connecting CNCs bundles with block copolymer chains. A reversible liquid-to-gel transition, triggered by temperature, was clearly detected by rheological measurements for the copolymer-CNC mixtures. At the optimal copolymer to CNC ratio the viscosity increased by 4 orders of magnitude at low shear rates. These stimuli-responsive CNC-based materials could be used as injectable biomedical systems.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2019
National Category
Other Chemistry Topics
Identifiers
urn:nbn:se:kth:diva-255395 (URN)10.1021/acs.biomac.9b00327 (DOI)000474812200009 ()31244017 (PubMedID)2-s2.0-85068116503 (Scopus ID)
Note

QC 20190729

Available from: 2019-07-29 Created: 2019-07-29 Last updated: 2019-10-04Bibliographically approved
Vilela, C., Engström, J., Valente, B. F. A., Jawerth, M., Carlmark, A. & Freire, C. S. R. (2018). Exploiting poly(ɛ-caprolactone) and cellulose nanofibrils modified with latex nanoparticles for the development of biodegradable nanocomposites. Polymer Composites
Open this publication in new window or tab >>Exploiting poly(ɛ-caprolactone) and cellulose nanofibrils modified with latex nanoparticles for the development of biodegradable nanocomposites
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2018 (English)In: Polymer Composites, ISSN 0272-8397, E-ISSN 1548-0569Article in journal (Refereed) Published
Abstract [en]

This study reports the development of nanocomposites based on poly(?-caprolactone) (PCL) and cellulose nanofibrils (CNF) modified with cationic latex nanoparticles. The physical adsorption of these water-based latexes on the surface of CNF was studied as an environment-friendly strategy to enhance the compatibility of CNF with a hydrophobic polymeric matrix. The latexes are composed of amphiphilic block copolymers based on cationic poly(N,N-dimethylaminoethyl methacrylate-co-methacrylic acid) as the hydrophilic block, and either poly(methyl methacrylate) or poly(n-butyl methacrylate) as the hydrophobic block. The simple and practical melt-mixing of PCL- and latex-modified CNF yielded white homogeneous nanocomposites with complete embedment of the nanofibrils in the thermoplastic matrix. All nanocomposites are semicrystalline materials with good mechanical properties (Young's modulus?=?43.6?52.3 MPa) and thermal stability up to 335?340°C. Degradation tests clearly showed that the nanocomposites slowly degrade in the presence of lipase-type enzyme. These PCL/CNF-latex nanocomposite materials show great promise as future environmentally friendly packaging materials. POLYM. COMPOS., 2018. ? 2018 Society of Plastics Engineers

Place, publisher, year, edition, pages
John Wiley & Sons, Ltd, 2018
National Category
Materials Chemistry
Identifiers
urn:nbn:se:kth:diva-241451 (URN)10.1002/pc.24865 (DOI)000463102200009 ()2-s2.0-85045412566 (Scopus ID)
Note

QC 20190123

Available from: 2019-01-22 Created: 2019-01-22 Last updated: 2019-04-29Bibliographically approved
Träger, A., Carlmark, A. & Wågberg, L. (2018). Interpenetrated Networks of Nanocellulose and Polyacrylamide with Excellent Mechanical and Absorptive Properties. Macromolecular materials and engineering (Print), 303(5), Article ID 1700594.
Open this publication in new window or tab >>Interpenetrated Networks of Nanocellulose and Polyacrylamide with Excellent Mechanical and Absorptive Properties
2018 (English)In: Macromolecular materials and engineering (Print), ISSN 1438-7492, E-ISSN 1439-2054, Vol. 303, no 5, article id 1700594Article in journal (Refereed) Published
Abstract [en]

Composites based on interpenetrating networks (IPNs) of cellulose nanofibril (CNF) aerogels and polyacrylamide are prepared and exhibit robust mechanical, water retaining, and re-swelling capacities. Furthermore, their swelling behavior is not affected by an increased ionic strength of the aqueous phase. These unprecedented IPNs combine the water retaining capacity of the polyacrylamide with the mechanical strength provided by the CNF aerogel template. The CNF aerogel/polyacrylamide composites exhibit a compressive stress at break greater than 250% compared with a neat polyacrylamide hydrogel. Furthermore, the composites retain their wet compression properties after drying and re-swelling, whereas the neat polyacrylamide hydrogels fail at a significantly lower stress and strain after drying and re-swelling. These composite materials highlight the potential of CNF aerogels to strengthen the mechanical properties and reduce the number of fracture defects during the drying and re-swelling of a hydrogel. These composites show the potential of being optimized for a plethora of applications, especially in the hygiene field and for biomedical devices.

Place, publisher, year, edition, pages
Wiley-VCH Verlagsgesellschaft, 2018
Keywords
CNF aerogels, composites, hydrogels, polyacrylamide
National Category
Composite Science and Engineering
Identifiers
urn:nbn:se:kth:diva-228438 (URN)10.1002/mame.201700594 (DOI)000432026700007 ()2-s2.0-85046904921 (Scopus ID)
Funder
Swedish Research Council
Note

QC 20180529

Available from: 2018-05-29 Created: 2018-05-29 Last updated: 2019-10-29Bibliographically approved
Engström, J., Hatton, F., Boujemaoui, A., Sanchez, C. C., Wågberg, L., D'Agosto, F., . . . Carlmark, A. (2018). Tailored nano-latexes for modification of nanocelluloses: Compatibilizing and plasticizing effects. Paper presented at 255th National Meeting and Exposition of the American-Chemical-Society (ACS) - Nexus of Food, Energy, and Water, MAR 18-22, 2018, New Orleans, LA. Abstract of Papers of the American Chemical Society, 255
Open this publication in new window or tab >>Tailored nano-latexes for modification of nanocelluloses: Compatibilizing and plasticizing effects
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2018 (English)In: Abstract of Papers of the American Chemical Society, ISSN 0065-7727, Vol. 255Article in journal, Meeting abstract (Other academic) Published
Place, publisher, year, edition, pages
American Chemical Society (ACS), 2018
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-240157 (URN)000435537702783 ()
Conference
255th National Meeting and Exposition of the American-Chemical-Society (ACS) - Nexus of Food, Energy, and Water, MAR 18-22, 2018, New Orleans, LA
Note

QC 20190111

Available from: 2019-01-11 Created: 2019-01-11 Last updated: 2019-01-11Bibliographically approved
Hatton, F., Engström, J., Forsling, J., Malmström, E. & Carlmark, A. (2017). Biomimetic adsorption of zwitterionic-xyloglucan block copolymers to CNF: towards tailored super-absorbing cellulose materials. RSC Advances, 7(24), 14947-14958
Open this publication in new window or tab >>Biomimetic adsorption of zwitterionic-xyloglucan block copolymers to CNF: towards tailored super-absorbing cellulose materials
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2017 (English)In: RSC Advances, ISSN 2046-2069, E-ISSN 2046-2069, Vol. 7, no 24, p. 14947-14958Article in journal (Refereed) Published
Abstract [en]

A biomimetic, facile approach to cellulose modification is the utilisation of self-adsorbing, naturally occurring biopolymers, such as the hemicellulose xyloglucan (XG). Herein, XG-block-poly(sulfobetaine methacrylate) (XG-b-PSBMA) zwitterionic block copolymers have been prepared and assessed for their ability to adsorb to cellulose, specifically cellulose nanofibrils (CNF). The polymers were synthesised using reversible addition-fragmentation chain-transfer (RAFT) polymerisation, employing an XG macromolecular RAFT agent (XG-RAFT), polymerising a sulfobetaine methacrylate (SBMA) under aqueous conditions. The incorporation of the XG block shifted the upper critical solution temperature (UCST) values to higher temperatures (20 and 30 °C) compared with the PSBMA homopolymers (17 and 22 °C) and the transition was also broadened. The adsorption of the polymers to a CNF surface was monitored using quartz crystal microbalance with dissipation monitoring (QCM-D), showing that the XG block enhanced the adsorption of the zwitterionic polymer. The formation of CNF-composite films was achieved utilising a facile vacuum filtration methodology, and the targeted compositions were confirmed by FT-IR and TGA analyses. The films exhibited high degrees of swelling in water, which were investigated at two different temperatures, 5 and 60 °C (below and above the polymer USCT values). These results highlight the advantage of using an XG block for the biomimetic modification of cellulose to form new cellulose-composite materials such as super-absorbing films.

Place, publisher, year, edition, pages
Royal Society of Chemistry, 2017
Keywords
Adsorption, Biomimetic materials, Biomimetics, Biopolymers, Block copolymers, Cellulose, Cellulose films, Composite films, Films, Free radical polymerization, Polymer films, Quartz crystal microbalances, Swelling, Biomimetic modification, Cellulose modifications, Macromolecular raft agents, Quartz crystal microbalance with dissipation monitoring, Reversible addition fragmentation chain transfer, Upper critical solution temperature, Zwitterionic block copolymers, Zwitterionic polymers, Polymers
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-207435 (URN)10.1039/c6ra28236a (DOI)000396150900075 ()2-s2.0-85014826088 (Scopus ID)
Note

QC 20170523

Available from: 2017-05-23 Created: 2017-05-23 Last updated: 2017-11-29Bibliographically approved
Hatton, F., Kedzior, S., Larsson, E., Cranston, E. & Carlmark, A. (2017). Grafting-from cellulose via photoinduced Cu-mediated reversible deactivation radical polymerisation. Paper presented at 253rd National Meeting of the American-Chemical-Society (ACS) on Advanced Materials, Technologies, Systems, and Processes, APR 02-06, 2017, San Francisco, CA. Abstract of Papers of the American Chemical Society, 253
Open this publication in new window or tab >>Grafting-from cellulose via photoinduced Cu-mediated reversible deactivation radical polymerisation
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2017 (English)In: Abstract of Papers of the American Chemical Society, ISSN 0065-7727, Vol. 253Article in journal, Meeting abstract (Other academic) Published
Place, publisher, year, edition, pages
American Chemical Society (ACS), 2017
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-243605 (URN)000430568503208 ()
Conference
253rd National Meeting of the American-Chemical-Society (ACS) on Advanced Materials, Technologies, Systems, and Processes, APR 02-06, 2017, San Francisco, CA
Note

QC 20190206

Available from: 2019-02-06 Created: 2019-02-06 Last updated: 2019-02-06Bibliographically approved
Boujemaoui, A., Sanchez, C. C., Engström, J., Bruce, C., Fogelström, L., Carlmark, A. & Malmström, E. (2017). Polycaprolactone Nanocomposites Reinforced with Cellulose Nanocrystals Surface-Modified via Covalent Grafting or Physisorption: A Comparative Study. ACS Applied Materials and Interfaces, 9(40), 35305-35318
Open this publication in new window or tab >>Polycaprolactone Nanocomposites Reinforced with Cellulose Nanocrystals Surface-Modified via Covalent Grafting or Physisorption: A Comparative Study
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2017 (English)In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 9, no 40, p. 35305-35318Article in journal (Refereed) Published
Abstract [en]

In the present work, cellulose nanocrystals (CNCs) have been surface-modified either via covalent grafting or through physisorption of poly(n-butyl methacrylate) (PBMA) and employed as reinforcement in PCL. Covalent grafting was achieved by surface-initiated atom transfer radical polymerization (SI-ATRP). Two approaches were utilized for the physisorption: using either micelles of poly(dimethyl aminoethyl methacrylate)-block-poly(n-butyl methacrylate) (PDMAEMA-b-PBMA) or latex nanoparticles of poly(dimethyl aminoethyl methacrylate-co-methacrylic acid)-block-poly(n-butyl methacrylate) (P(DMAEMA-co-MAA)-b-PBMA). Block copolymers (PDMAEMA-b-PBMA)s were obtained by ATRP and subsequently micellized. Latex nanoparticles were produced via reversible addition-fragmentation chain-transfer (RAFT) mediated surfactant-free emulsion polymerization, employing polymer-induced self-assembly (PISA) for the particle formation. For a reliable comparison, the amounts of micelles/latex particles adsorbed and the amount of polymer grafted onto the CNCs were kept similar. Two different chain lengths of PBMA were targeted, below and above the critical molecular weight for chain entanglement of PBMA (M-n,M-c similar to 56 000 g mo1(-1)). Poly(epsilon-caprolactone) (PCL) nanocomposites reinforced with unmodified and modified CNCs in different weight percentages (0.5, 1, and 3 wt %) were prepared via melt extrusion. The resulting composites were evaluated by UV-vis, scanning electron microscopy (SEM), thermal gravimetric analysis (TGA), and tensile testing. All materials resulted in higher transparency, greater thermal stability, and stronger mechanical properties than unfilled PCL and nanocomposites containing unmodified CNCs. The degradation temperature of PCL reinforced with grafted CNCs was higher than that of micelle-modified CNCs, and the latter was higher than that of latex-adsorbed CNCs with a long PBMA chain length. The results clearly indicate that covalent grafting is superior to physisorption with regard to thermal and mechanical properties of the final nanocomposite. This unique study is of great value for the future design of CNC-based nanocomposites with tailored properties.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2017
Keywords
cellulose nanocrystals (CNCs), covalent grafting physisorption, reversible-deactivation radical polymerization (RDRP), poly(epsilon-caprolactone) (PCL), nanocomposites
National Category
Other Chemistry Topics
Identifiers
urn:nbn:se:kth:diva-217193 (URN)10.1021/acsami.7b09009 (DOI)000413131500079 ()28895728 (PubMedID)2-s2.0-85031302620 (Scopus ID)
Funder
Swedish Foundation for Strategic Research , EM11-0022
Note

QC 20171102

Available from: 2017-11-02 Created: 2017-11-02 Last updated: 2019-01-23Bibliographically approved
Gicquel, E., Jean, B., Engström, J., Martin, C., Carlmark, A. & Bras, J. (2017). Rheological behavior of thermosensitive hydrogel suspensions based on Cellulose Nanocrystals with adsorbed thermo-responsive polymer. Paper presented at 253rd National Meeting of the American-Chemical-Society (ACS) on Advanced Materials, Technologies, Systems, and Processes, APR 02-06, 2017, San Francisco, CA. Abstract of Papers of the American Chemical Society, 253
Open this publication in new window or tab >>Rheological behavior of thermosensitive hydrogel suspensions based on Cellulose Nanocrystals with adsorbed thermo-responsive polymer
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2017 (English)In: Abstract of Papers of the American Chemical Society, ISSN 0065-7727, Vol. 253Article in journal, Meeting abstract (Other academic) Published
Place, publisher, year, edition, pages
American Chemical Society (ACS), 2017
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-243603 (URN)000430568503300 ()
Conference
253rd National Meeting of the American-Chemical-Society (ACS) on Advanced Materials, Technologies, Systems, and Processes, APR 02-06, 2017, San Francisco, CA
Note

QC 20190206

Available from: 2019-02-06 Created: 2019-02-06 Last updated: 2019-02-06Bibliographically approved
Organisations
Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0002-8194-0058

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