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Koo, J. M., Kang, J., Shin, S.-H., Jegal, J., Cha, H. G., Choy, S., . . . Hwang, S. Y. (2020). Biobased thermoplastic elastomer with seamless 3D-Printability and superior mechanical properties empowered by in-situ polymerization in the presence of nanocellulose. Composites Science And Technology, 185, Article ID 107885.
Open this publication in new window or tab >>Biobased thermoplastic elastomer with seamless 3D-Printability and superior mechanical properties empowered by in-situ polymerization in the presence of nanocellulose
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2020 (English)In: Composites Science And Technology, ISSN 0266-3538, E-ISSN 1879-1050, Vol. 185, article id 107885Article in journal (Refereed) Published
Abstract [en]

A biobased and biocompatible thermoplastic elastomer (TPE) with superior 3D printability was demonstrated with great potential for customized manufacturing technologies and fabrication of biointegrated devices. The inherent structural and stereochemical disadvantages of biobased monomers, such as 2,5-furandicarboxylic acid, in comparison with today used petroleum based monomers like terephthalic acid generally lead to lower mechanical performance for the biobased replacement polymers. This is additionally enhanced by poor interfacial adhesion and fusion commonly encountered during customized manufacturing technologies like 3D printing. Herein, we demonstrate that in-situ polymerization in the presence of trace amounts of cellulose nanocrystals (CNCs) can homogeneously distribute the nanofiller leading to dramatically strengthened thermally 3D-printable bio-furan-based TPE. This TPE exhibited a tensile strength of 67 MPa which is 1.5-7-fold higher than the values reported for silicone and thermoplastic urethane, which are widely used in biomedical applications. In addition, the TPE had an impressive extensibility of 860% and negligible in vivo cytotoxicity; such properties have not been reported to date for bio-based or petrochemical TPEs. While a petrochemical 3D printed TPE counterpart retained only half of the tensile strength compared to the hot-pressed analogue, the 3D-printed biobased TPE insitu modified with nanocellulose maintained 70-80% of its strength under the same experimental conditions. This is explained by inter-diffusion between interfaces facilitated by the nanocellulose and the furan rings. Using the ergonomic shape of a wrist as a 3D-printable design, we successfully manufactured a wearable thermal therapeutic device from the nanocellulose modified biobased TPE, giving promise for wide variety of future applications.

Place, publisher, year, edition, pages
ELSEVIER SCI LTD, 2020
Keywords
Polymers, Flexible composite, Nano composites, Mechanical properties, 3D-printing
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-266425 (URN)10.1016/j.compscitech.2019.107885 (DOI)000503090500001 ()2-s2.0-85074799210 (Scopus ID)
Note

QC 20200121

Available from: 2020-01-21 Created: 2020-01-21 Last updated: 2020-01-21Bibliographically approved
Yadav, A., Benyahia Erdal, N., Hakkarainen, M., Nandan, B. & Srivastava, V. (2020). Cellulose-Derived Nanographene Oxide Reinforced Macroporous Scaffolds of High Internal Phase Emulsion-Templated Cross-Linked Poly(ϵ-caprolactone). Biomacromolecules, 21(2), 589-596
Open this publication in new window or tab >>Cellulose-Derived Nanographene Oxide Reinforced Macroporous Scaffolds of High Internal Phase Emulsion-Templated Cross-Linked Poly(ϵ-caprolactone)
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2020 (English)In: Biomacromolecules, ISSN 1525-7797, E-ISSN 1526-4602, Vol. 21, no 2, p. 589-596Article in journal (Refereed) Published
Abstract [en]

Cellulose-derived nanographene oxide (nGO)-type carbon dot reinforced porous scaffolds of poly(epsilon-caprolactone) (PCL) were developed as templates from high internal phase emulsions (HIPE). The mechanical strength, structural integrity, and reusability of the scaffolds were enhanced via in situ cross-linking. An oil-in-oil (o/o) HIPE of epsilon-caprolactone monomer (CL) was made for this purpose, and the ring-opening polymerization of a continuous phase comprised of CL, catalyst (Sn(Oct)(2)), and cross-linker (bis(caprolactone-4-yl)) (BCY) was carried out. The functionalization of scaffolds with nGO was assessed along with its role as an effective Pickering stabilizer of the HIPEs. The pore size and porosity of the scaffolds were governed by HIPE morphology, which in turn was controlled by the amount of nGO and the volume fraction of the dispersed phase. The nGO-functionalized scaffolds of cross-linked PCL thus prepared were characterized for their morphological structure, mechanical strength, and oil sorption capacity. Enhanced oil adsorption of nGO-functionalized scaffolds proved them to be of higher potency compared to those made of neat PCL. Superior compressive strength and reusability of scaffolds for oil adsorption up to 40 times while maintaining the structural integrity for >= 25 sorption-desorption cycles added extra value to such scaffolds. The scaffolds also had excellent cell viability as evaluated by MG63 osteoblast-like cells and some bioactivity in the form of calcium phosphate mineralization on the surface of the scaffolds.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2020
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-267849 (URN)10.1021/acs.biomac.9b01330 (DOI)000513091100030 ()31830781 (PubMedID)2-s2.0-85077697992 (Scopus ID)
Note

QC 20200306

Available from: 2020-03-06 Created: 2020-03-06 Last updated: 2020-03-16Bibliographically approved
Rahimi-Aghdam, T., Shariatinia, Z., Hakkarainen, M. & Haddadi-Asl, V. (2020). Nitrogen and phosphorous doped graphene quantum dots: Excellent flame retardants and smoke suppressants for polyacrylonitrile nanocomposites. Journal of Hazardous Materials, 381, Article ID 121013.
Open this publication in new window or tab >>Nitrogen and phosphorous doped graphene quantum dots: Excellent flame retardants and smoke suppressants for polyacrylonitrile nanocomposites
2020 (English)In: Journal of Hazardous Materials, ISSN 0304-3894, E-ISSN 1873-3336, Vol. 381, article id 121013Article in journal (Refereed) Published
Abstract [en]

Nitrogen (N-GQD) as well as nitrogen and phosphorous co-doped (NP-GQD) graphene quantum dots were demonstrated as novel, low cost, green and highly effective flame retardants and smoke suppressants for polyacrylonitrile (PAN) nanocomposites. The N-GQD and NP-GQD samples were synthesized by hydrothermal method with citric acid as the main reactant. For the first time, the flame retardant and smoke suppressant properties of the NP-GQD were studied. The GQDs were introduced into PAN by solvent blending route. Subsequently, thermal stability, flame retardancy, fire behavior, fire hazard and structure of the residual char were investigated by thermogravimetric analysis (TGA), UL-94 vertical burning test, cone calorimetry, FE-SEM, and Raman spectroscopy. Results showed that both PAN/N-GQD and PAN/NP-GQD nanocomposites had higher flame retardancy and smoke suppressant behavior in addition to lower fire hazard properties than neat PAN. Furthermore, the residual chars for the nanocomposite samples were increased in comparison to the neat PAN. The improvements were even more significant in case of the PAN/NP-GQD due to the synergistic effect of nitrogen and phosphorous. The improvements were mainly ascribed to the ability of the N-GQD and NP-GQD to provide stronger and larger protective char barrier layers, which was even more pronounced in case of the NP-GQD.

Place, publisher, year, edition, pages
Elsevier, 2020
Keywords
Char barrier layer, Fire hazard, Flame retardant, N and P co-doped graphene quantum dot (NP-GQD), Polyacrylonitrile (PAN), Smoke suppressant
National Category
Polymer Technologies
Research subject
Fibre and Polymer Science; Physics, Material and Nano Physics
Identifiers
urn:nbn:se:kth:diva-263435 (URN)10.1016/j.jhazmat.2019.121013 (DOI)000504778400072 ()31442693 (PubMedID)2-s2.0-85070915285 (Scopus ID)
Note

QC 20191205

Available from: 2019-12-05 Created: 2019-12-05 Last updated: 2020-03-09Bibliographically approved
Golda-Cepa, M., Engvall, K., Hakkarainen, M. & Kotarba, A. (2020). Recent progress on parylene C polymer for biomedical applications: A review. Progress in organic coatings, 140, Article ID 105493.
Open this publication in new window or tab >>Recent progress on parylene C polymer for biomedical applications: A review
2020 (English)In: Progress in organic coatings, ISSN 0300-9440, E-ISSN 1873-331X, Vol. 140, article id 105493Article, review/survey (Refereed) Published
Abstract [en]

Parylene C films have numerous advantages. The versatility of parylene C coatings makes them useful in a broad range of biomedical applications. The coatings are widely used commercially because of the unique combination of their physicochemical properties, i.e. flexibility and dielectricity. The chemical vapour deposition process enables parylene C conformal coatings to be applied to even the most complex medical devices. The coatings can be customised for the desired application using surface modification methods, which alter surface chemistry and topography. In this review, we summarise the last ten years (2008–2018) of research on parylene C for biomedical applications. We discuss how parylene C properties can be modulated through surface and bulk modifications to improve its key functions, i.e. anticorrosive, biocompatible, anti-infection, and therapeutic functions. We emphasise current and potential biomedical applications and finally highlight the advantages and limitations of the coatings, pointing out the perspectives and the most promising research trends.

Place, publisher, year, edition, pages
Elsevier, 2020
Keywords
Biocompatibility, Biomaterial, Biomedical coating, CVD, Parylene C, Surface functionalisation
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-267799 (URN)10.1016/j.porgcoat.2019.105493 (DOI)2-s2.0-85076429770 (Scopus ID)
Note

QC 20200304

Available from: 2020-03-04 Created: 2020-03-04 Last updated: 2020-03-04Bibliographically approved
Pronoitis, C., Hua, G., Hakkarainen, M. & Odelius, K. (2019). Biobased Polyamide Thermosets: From a Facile One-Step Synthesis to Strong and Flexible Materials. Macromolecules, 52(16), 6181-6191
Open this publication in new window or tab >>Biobased Polyamide Thermosets: From a Facile One-Step Synthesis to Strong and Flexible Materials
2019 (English)In: Macromolecules, ISSN 0024-9297, E-ISSN 1520-5835, Vol. 52, no 16, p. 6181-6191Article in journal (Refereed) Published
Abstract [en]

Biobased polyamide (PA) thermosets composed of renewable ethylene brassylate were synthesized through a one-step reaction under solvent-free conditions, at 100 degrees C in the presence of an organocatalyst. Under these conditions, thermoset formation times as low as 10 min were achieved. The thermosets were easily prepared as thin, transparent films with high strength, flexibility, and high thermal stability. The ester-to-amine content and formation of ethylene glycol in situ as a byproduct of the reaction were studied and correlated with the final properties of the materials. Crystalline oligoester segments were identified as a result of ring-opening polymerization and were shown to have a beneficial effect on the mechanical properties of the thermosets and endowed shape-memory behavior. In contrast to other routes, employing multistep monomer preparation, harsh conditions, and chlorinated reagents, this procedure contributed to the development of sustainable, functional PA thermosets.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC, 2019
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-260186 (URN)10.1021/acs.macromol.9b00359 (DOI)000483437500015 ()2-s2.0-85071380280 (Scopus ID)
Note

QC 20190930

Available from: 2019-09-30 Created: 2019-09-30 Last updated: 2019-09-30Bibliographically approved
Hakkarainen, M. (2019). Carbon dots as bioactivity inducers in polymeric biomaterials. Paper presented at National Meeting of the American-Chemical-Society (ACS), MAR 31-APR 04, 2019, Orlando, FL. Abstracts of Papers of the American Chemical Society, 257
Open this publication in new window or tab >>Carbon dots as bioactivity inducers in polymeric biomaterials
2019 (English)In: Abstracts of Papers of the American Chemical Society, ISSN 0065-7727, Vol. 257Article in journal, Meeting abstract (Other academic) Published
Place, publisher, year, edition, pages
AMER CHEMICAL SOC, 2019
National Category
Paper, Pulp and Fiber Technology
Identifiers
urn:nbn:se:kth:diva-257607 (URN)000478860502765 ()
Conference
National Meeting of the American-Chemical-Society (ACS), MAR 31-APR 04, 2019, Orlando, FL
Note

QC 20190919

Available from: 2019-09-19 Created: 2019-09-19 Last updated: 2019-11-12Bibliographically approved
Gazzotti, S., Rampazzo, R., Hakkarainen, M., Bussini, D., Ortenzi, M. A., Farina, H., . . . Silvani, A. (2019). Cellulose nanofibrils as reinforcing agents for PLA-based nanocomposites: An in situ approach. Composites Science And Technology, 171, 94-102
Open this publication in new window or tab >>Cellulose nanofibrils as reinforcing agents for PLA-based nanocomposites: An in situ approach
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2019 (English)In: Composites Science And Technology, ISSN 0266-3538, E-ISSN 1879-1050, Vol. 171, p. 94-102Article in journal (Refereed) Published
Abstract [en]

One-pot in situ polymerization approach was explored for the preparation of polylactide (PLA)-cellulose nano-fibril (CNF) bio-nanocomposites. CNF were first prepared through enzymatic and mechanical treatment of bleached hardwood kraft pulp. The bio-nanocomposites- were then fabricated through ring opening polymerization (ROP) of L-lactide, in the presence of various amounts of fibrils. Molecular weight, thermal properties, surface morphology, mechanical and wettability properties of the PLA-CNF nanocomposites were evaluated. DSC analysis demonstrated the effect of CNF on crystallization and crystalline morphology of PLA. Improved modulus for the nanocomposites with respect to standard PLA was demonstrated, however, the differences in tensile stress were small probably due to the counteracting effects of reinforcement from CNF and the decreasing molecular weight as a function of CNF concentration. The absence of pulled-out fibers was assessed, highlighting the strong interface and covalent attachment of PLA chains on CNF surface. Finally, the covalent bonding of PLA chains on CNF surface was demonstrated by isolating the non-soluble part, consisting of PLA-grafted CNF, and characterization of this residue.

Place, publisher, year, edition, pages
ELSEVIER SCI LTD, 2019
Keywords
Fibers, Nano composites, Polymers, Short-fibre composites, Interfacial strength
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-244094 (URN)10.1016/j.compscitech.2018.12.015 (DOI)000457505600011 ()2-s2.0-85058640232 (Scopus ID)
Note

QC 20190219

Available from: 2019-02-19 Created: 2019-02-19 Last updated: 2019-02-19Bibliographically approved
Erdal, N. B., Yao, J. G. & Hakkarainen, M. (2019). Cellulose-Derived Nanographene Oxide Surface-Functionalized Three-Dimensional Scaffolds with Drug Delivery Capability. Paper presented at Symposium on Rational Design of Multifunctional Renewable-Resourced Materials held during the ACS National Meeting, AUG 19-23, 2018, Boston, MA. Biomacromolecules, 20(2), 738-749
Open this publication in new window or tab >>Cellulose-Derived Nanographene Oxide Surface-Functionalized Three-Dimensional Scaffolds with Drug Delivery Capability
2019 (English)In: Biomacromolecules, ISSN 1525-7797, E-ISSN 1526-4602, Vol. 20, no 2, p. 738-749Article in journal (Refereed) Published
Abstract [en]

Multifunctional three-dimensional (3D) scaffolds were targeted by surface grafting cellulose-derived nanographene oxide (nGO) on the surface of porous poly(epsilon-caprolactone) (PCL) scaffolds. nGO was derived from cellulose by microwave-assisted carbonization process and covalently grafted onto aminolyzed PCL scaffolds through an aqueous solution process. Fourier transform infrared spectroscopy and thermogravimetric analysis both verified the successful attachment of nGO and scanning electron microscopy depicted a homogeneous dispersion of nGO over the scaffold surface. Mechanical tests were performed and demonstrated a significant increase in compressive strength for the nGO grafted scaffolds. Grafting of nGO was also shown to induce mineralization with the formation of calcium phosphate precipitates on the surface of the scaffolds with the size increasing with higher nGO content. The potential of surface-grafted nGO as a nanocarrier of an antibiotic drug was also explored. The secondary interactions between nGO and ciprofloxacin, a broad-spectrum antibiotic used in the treatment of osteomyelitis, were optimized by controlling the solution pH. Ciprofloxacin was found to be adsorbed most strongly in its cationic form at pH 5, in which pi-pi electron donor-acceptor interactions predominate and the adsorbed drug content increased with increasing nGO amount. Further, the release kinetics of the drug were investigated during 8 days. In conclusion, the proposed simple fabrication process led to a scaffold with multifunctionality in the form of improved mechanical strength, ability to induce mineralization, as well as drug loading and delivery capability.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2019
National Category
Biochemistry and Molecular Biology
Identifiers
urn:nbn:se:kth:diva-245945 (URN)10.1021/acs.biomac.8b01421 (DOI)000458937200017 ()30360619 (PubMedID)2-s2.0-85056460762 (Scopus ID)
Conference
Symposium on Rational Design of Multifunctional Renewable-Resourced Materials held during the ACS National Meeting, AUG 19-23, 2018, Boston, MA
Note

QC 20190313

Available from: 2019-03-13 Created: 2019-03-13 Last updated: 2019-03-13Bibliographically approved
Bäckström, E., Odelius, K. & Hakkarainen, M. (2019). Designed from Recycled: Turning Polyethylene Waste to Covalently Attached Polylactide Plasticizers. ACS SUSTAINABLE CHEMISTRY & ENGINEERING, 7(12), 11004-11013
Open this publication in new window or tab >>Designed from Recycled: Turning Polyethylene Waste to Covalently Attached Polylactide Plasticizers
2019 (English)In: ACS SUSTAINABLE CHEMISTRY & ENGINEERING, ISSN 2168-0485, Vol. 7, no 12, p. 11004-11013Article in journal (Refereed) Published
Abstract [en]

High-density polyethylene (HDPE) waste was successfully feedstock recycled, and the obtained chemicals were utilized for synthesis of plasticizers for polylactide (PLA). First, an effective route to recycle HDPE through a microwave-assisted hydrothermal process was established. This process led to selective degradation of HDPE to a few well-defined chemicals, namely, succinic, glutaric, and adipic acid. A model plasticizer was synthesized from the same composition of dicarboxylic acids, 1,4-butanediol, and crotonic acid. The function of crotonic acid was to produce oligomers with crotonate end groups for coupling the plasticizer to PLA main chain. The plasticizer was then blended with or coupled to PLA by a reactive extrusion process. Adding the plasticizer to PLA decreased the T-g and increased the strain at break, thus reducing the brittleness of the films. The addition of 20% (w/w) grafted plasticizer increased the strain at break of PLA from 6 to 156% and decreased the T-g by 15 degrees C compared with neat PLA. Finally, to verify the concept, a plasticizer was also synthesized from the dicarboxylic acid product mixture obtained from the feedstock recycling of HDPE. The recycled grafted plasticizer increased the strain at break of PLA to 142% and reduced the T-g by 10 degrees C. A promising route for designing from recycled feedstock, turning HDPE waste to PLA plasticizers, was thus demonstrated.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC, 2019
Keywords
HDPE, Oxidative degradation, Feedstock recycling, PLA, Plasticization
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-255190 (URN)10.1021/acssuschemeng.9b02092 (DOI)000472240900091 ()2-s2.0-85067031627 (Scopus ID)
Note

QC 20190904

Available from: 2019-09-04 Created: 2019-09-04 Last updated: 2019-09-04Bibliographically approved
Delekta, S. S., Adolfsson, K. H., Benyahia Erdal, N., Hakkarainen, M., Östling, M. & Li, J. (2019). Fully inkjet printed ultrathin microsupercapacitors based on graphene electrodes and a nano-graphene oxide electrolyte. Nanoscale, 11(21), 10172-10177
Open this publication in new window or tab >>Fully inkjet printed ultrathin microsupercapacitors based on graphene electrodes and a nano-graphene oxide electrolyte
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2019 (English)In: Nanoscale, ISSN 2040-3364, E-ISSN 2040-3372, Vol. 11, no 21, p. 10172-10177Article in journal (Refereed) Published
Abstract [en]

The advance of miniaturized and low-power electronics has a striking impact on the development of energy storage devices with constantly tougher constraints in terms of form factor and performance. Microsupercapacitors (MSCs) are considered a potential solution to this problem, thanks to their compact device structure. Great efforts have been made to maximize their performance with new materials like graphene and to minimize their production cost with scalable fabrication processes. In this regard, we developed a full inkjet printing process for the production of all-graphene microsupercapacitors with electrodes based on electrochemically exfoliated graphene and an ultrathin solid-state electrolyte based on nano-graphene oxide. The devices exploit the high ionic conductivity of nano-graphene oxide coupled with the high electrical conductivity of graphene films, yielding areal capacitances of up to 313 mu F cm-2 at 5 mV s-1 and high power densities of up to 4 mW cm-3 with an overall device thickness of only 1 mu m.

Place, publisher, year, edition, pages
Royal Society of Chemistry, 2019
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-254076 (URN)10.1039/c9nr01427f (DOI)000470697800002 ()31107494 (PubMedID)2-s2.0-85066626832 (Scopus ID)
Note

QC 20190624

Available from: 2019-06-24 Created: 2019-06-24 Last updated: 2019-08-16Bibliographically approved
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ORCID iD: ORCID iD iconorcid.org/0000-0002-7790-8987

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