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Benyahia Erdal, N., Adolfsson, K. H., Pettersson, T. & Hakkarainen, M. (2018). Green Strategy to Reduced Nanographene Oxide through Microwave Assisted Transformation of Cellulose. ACS Sustainable Chemistry and Engineering, 6(1), 1245-1255.
Open this publication in new window or tab >>Green Strategy to Reduced Nanographene Oxide through Microwave Assisted Transformation of Cellulose
2018 (English)In: ACS Sustainable Chemistry and Engineering, ISSN 2168-0485, Vol. 6, no 1, 1245-1255 p.Article in journal (Refereed) Published
Abstract [en]

A green strategy for fabrication of biobased reduced nanographene oxide (r-nGO) was developed. Cellulose derived nanographene oxide (nGO) type carbon nanodots were reduced by microwave assisted hydrothermal treatment with superheated water alone or in the presence of caffeic acid (CA), a green reducing agent. The carbon nanodots, r-nGO and r-nGO-CA, obtained through the two different reaction routes without or with the added reducing agent, were characterized by multiple analytical techniques including FTIR, XPS, Raman, XRD, TGA, TEM, AFM, UV-vis, and DLS to confirm and evaluate the efficiency of the reduction reactions. A significant decrease in oxygen content accompanied by increased number of sp2 hybridized functional groups was confirmed in both cases. The synergistic effect of superheated water and reducing agent resulted in the highest C/O ratio and thermal stability, which also supported a more efficient reduction. Interesting optical properties were detected by fluorescence spectroscopy where nGO, r-nGO, and r-nGO-CA all displayed excitation dependent fluorescence behavior. r-nGO-CA and its precursor nGO were evaluated toward osteoblastic cells MG-63 and exhibited nontoxic behavior up to 200 μg mL-1, which gives promise for utilization in biomedical applications.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2018
Keyword
Biobased, Biomass, Carbon nanodots, Hydrothermal, Microwave, Reducing agent
National Category
Other Chemical Engineering
Identifiers
urn:nbn:se:kth:diva-221151 (URN)10.1021/acssuschemeng.7b03566 (DOI)2-s2.0-85040200237 (Scopus ID)
Note

QC 20180115

Available from: 2018-01-15 Created: 2018-01-15 Last updated: 2018-01-15Bibliographically approved
Feng, Z., Simeone, A., Odelius, K. & Hakkarainen, M. (2017). Biobased Nanographene Oxide Creates Stronger Chitosan Hydrogels with Improved Adsorption Capacity for Trace Pharmaceuticals. ACS Sustainable Chemistry & Engineering, 5(12), 11525-11535.
Open this publication in new window or tab >>Biobased Nanographene Oxide Creates Stronger Chitosan Hydrogels with Improved Adsorption Capacity for Trace Pharmaceuticals
2017 (English)In: ACS Sustainable Chemistry & Engineering, ISSN 2168-0485, Vol. 5, no 12, 11525-11535 p.Article in journal (Refereed) Published
Abstract [en]

A promising green strategy for the fabrication of fully biobased chitosan adsorbents for wastewater purification is presented. Nanographene oxide (nGO)-type carbon dots were derived from chitosan (nGOCS) or from cellulose (nGOCL) through a two-step process including microwave-assisted hydrothermal carbonization and oxidation. Finally, nGO were evaluated as biobased property enhancers in chitosan hydrogel adsorbents. Macroporous chitosan hydrogels were synthesized by cross-linking with genipin, and the incorporation of nGO into these hydrogels was shown to facilitate the cross-linking reaction leading to more robust 3D cross-linked networks. This was evidenced by the increased storage modulus and by the swelling ratio that decreased from 5.7 for pristine chitosan hydrogel to 2.6 for hydrogel with 5 mg/mL nGOCS and 3.3 for hydrogel with 5 mg/mL nGOCL. As a further proof of the concept the hydrogels were shown to be effective adsorbent for the common anti-inflammatory drug diclofenac sodium (DCF). Here, the addition of nGO promoted the DCF adsorption process leading to 100% removal of DCF after only 5 h. The synergistic effect of electrostatic interactions, hydrogen bonding, and pi-pi stacking could explain the high adsorption of DCF on the hydrogels. The developed biobased CS/nGO hydrogels are thus promising adsorbents with great potential for purification of trace pharmaceuticals from wastewater.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2017
Keyword
Graphene oxide, Carbon dot, Hydrogel, Diclofenac sodium, Genipin, Microwave, Waste water purification, Adsorbent
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-220462 (URN)10.1021/acssuschemeng.7b02809 (DOI)000417341900044 ()
Note

QC 20171221

Available from: 2017-12-21 Created: 2017-12-21 Last updated: 2017-12-21Bibliographically approved
Xu, H., Xie, L., Li, J. & Hakkarainen, M. (2017). Coffee Grounds to Multifunctional Quantum Dots: Extreme Nanoenhancers of Polymer Biocomposites. ACS Applied Materials and Interfaces, 9(33), 27972-27983.
Open this publication in new window or tab >>Coffee Grounds to Multifunctional Quantum Dots: Extreme Nanoenhancers of Polymer Biocomposites
2017 (English)In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 9, no 33, 27972-27983 p.Article in journal (Refereed) Published
Abstract [en]

Central to the design and execution of nanocomposite strategies is the invention of polymer-affinitive and multifunctional nanoreinforcements amenable to economically viable processing. Here, a microwave-assisted approach enabled gram-scale fabrication of polymer-affinitive luminescent quantum dots (QDs) from spent coffee grounds. The ultrasmall dimensions (approaching 20 nm), coupled with richness of diverse oxygen functional groups, conferred the zero-dimensional QDs with proper exfoliation and uniform dispersion in poly(L-lactic acid) (PLLA) matrix The unique optical properties of QDs were inherited by PLLA nano composites, giving intensive luminescence and high visible transparency, as well as nearly 100% UV-blocking ratio in the full-UV region at only 0.5 wt % QDs. The strong anchoring of PLLA chains at the nanoscale surfaces of QDs facilitated PLLA crystallization, which was accompanied by substantial improvements in thermomechanical and tensile properties. With 1 wt % QDs, for example, the storage modulus at 100 degrees C and tensile strength increased over 2500 and 69% compared to those of pure PLLA (4 and 57.3 MPa), respectively. The QD-enabled energy-dissipating and flexibility-imparting mechanisms upon tensile deformation, including the generation of numerous shear bands, crazing, and nanofibrillation, gave an unusual combination of elasticity and extensibility for PLLA nanocomposites. This paves the way to biowaste-derived nanodots with high affinity to polymer for elegant implementation of distinct light management and extreme nanoreinforcements in an ecofriendly manner.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2017
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-214503 (URN)10.1021/acsami.7b09401 (DOI)000408518800070 ()28770986 (PubMedID)2-s2.0-85028084609 (Scopus ID)
Note

QC 20170929

Available from: 2017-09-29 Created: 2017-09-29 Last updated: 2017-09-29Bibliographically approved
Albertsson, A.-C. & Hakkarainen, M. (2017). Designed to degrade Suitably designed degradable polymers can play a role in reducing plastic waste. Science, 358(6365), 872-873.
Open this publication in new window or tab >>Designed to degrade Suitably designed degradable polymers can play a role in reducing plastic waste
2017 (English)In: Science, ISSN 0036-8075, E-ISSN 1095-9203, Vol. 358, no 6365, 872-873 p.Article in journal, Editorial material (Refereed) Published
Place, publisher, year, edition, pages
American Association for the Advancement of Science, 2017
National Category
Polymer Technologies
Identifiers
urn:nbn:se:kth:diva-219332 (URN)10.1126/science.aap8115 (DOI)000415293000027 ()29146799 (PubMedID)
Note

QC 20171204

Available from: 2017-12-04 Created: 2017-12-04 Last updated: 2017-12-04Bibliographically approved
Michalak, M., Kwiecien, I., Kwiecien, M., Adamus, G., Odelius, K., Hakkarainen, M. & Kurcok, P. (2017). Diversifying Polyhydroxyalkanoates - End-Group and Side-Chain Functionality. Current Organic Synthesis, 14(6), 757-767.
Open this publication in new window or tab >>Diversifying Polyhydroxyalkanoates - End-Group and Side-Chain Functionality
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2017 (English)In: Current Organic Synthesis, ISSN 1570-1794, E-ISSN 1875-6271, Vol. 14, no 6, 757-767 p.Article, review/survey (Refereed) Published
Abstract [en]

Background: Polyhydroxyalkanoates (PHAs) are a natural origin biodegradable polyesters consisted of various 3-and 4-hydroxyacid derived repeating units produced by microorganisms as energy storage. PHAs have been intensively studied due to their biodegradability and biocompatibility enabling their use both in packaging and agriculture as well as in medicine and pharmacy. PHAs obtained via biotechnological routes can possess various functional groups in their side chains. However, the diversity in their functionality is limited due to issues of conservation of functional groups during the polymer formation. Objective: The review focuses on recent progress in the area of synthesis of PHAs functionalized with various reactive as well as bioactive end and side groups. Conclusion: A potent route to resolve the problem of functional group diversity in natural origin PHAs involves post-polymerization modification, where the desired side groups can be created. On the contrary, synthetically produced PHA analogs obtained directly via ring-opening polymerization of beta-lactones offer various functionalities at different position throughout the polymer chain. The desired alpha-and omega-end groups can be introduced into the polymer chain using specific polymerization, initiation or termination strategies, respectively. The preferred side chain functionality is obtained by choosing the appropriate beta-lactone monomers bearing respective functional groups. All functional groups may also be subjected to additional chemical modification. The degradation of PHA as a method for producing functional polymers as well as their possible further applications are also discussed.

Keyword
Polyesters, polyhydroxyalkanoates, poly(3-hydroxybutyrate), functional polymer, ring-opening polymerization, side-chain functionalization, reactive end groups
National Category
Polymer Technologies
Identifiers
urn:nbn:se:kth:diva-220305 (URN)10.2174/1570179414666161115150146 (DOI)000416527500002 ()
Note

QC 20171221

Available from: 2017-12-21 Created: 2017-12-21 Last updated: 2017-12-21Bibliographically approved
Xu, H., Bai, Y., Xie, L., Li, J. & Hakkarainen, M. (2017). Heat-Resistant and Microwaveable Poly(Iactic acid) by Quantum-Dot Promoted Stereocomplexation. ACS Sustainable Chemistry & Engineering, 5(12), 11607-11617.
Open this publication in new window or tab >>Heat-Resistant and Microwaveable Poly(Iactic acid) by Quantum-Dot Promoted Stereocomplexation
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2017 (English)In: ACS Sustainable Chemistry & Engineering, ISSN 2168-0485, Vol. 5, no 12, 11607-11617 p.Article in journal (Refereed) Published
Abstract [en]

Nanofiller-tailored stereocomplexation signifies a promising and feasible pathway to develop heat-resistant poly (lactic acid) (PLA) materials. However, this pathway is thwarted by the potential adverse environmental issues of traditional nanofillers and the challenges in facilitating the nanofiller dispersion and selective formation of stereocomplex crystals (SCs). Here we unravel a microwave-assisted approach to exploit biobased quantum dots (QDs) featuring excellent capability to preferably nucleate PLA SCs. The combination of ultrasmall dimension and high oxygenation degree of QDs conferred intimate interactions with stereocomplexed PLA chains, readying complete exfoliation and uniform dispersion of QDs to promote stereocomplexation. The well-dispersed QDs provided perfect UV shielding for PLA composites, while sustaining high transmission to visible light comparable to pure PLA. Strong interfacial interactions and high concentration of SCs were created around the nanoscale surfaces of QDs, accounting for the greatly increased resistance to oxygen permeation, thermal deformation, and microwave heating. This was accompanied by substantial rise in tensile modulus and elongation at break (up to 74 and 51%) compared to that of pure PLA, affording the demonstration of unusual reinforcing and toughening mechanisms imparted by the PLA-affinitive QDs. The robust structural integrity under harsh usage environments, coupled with high gas barrier, prominent light management and evasion of flexibility and extensibility sacrifices, may prompt low-cost and ecofriendly PLA nanocomposites suitable for diverse applications including microwaveable food packaging.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2017
Keyword
polylactide, stereocomplex, quantum dots, UV shielding, thermal resistance, microwaveable packaging
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-220463 (URN)10.1021/acssuschemeng.7b02963 (DOI)000417341900053 ()
Note

QC 20180103

Available from: 2018-01-03 Created: 2018-01-03 Last updated: 2018-01-03Bibliographically approved
Michalak, M., Kurcok, P. & Hakkarainen, M. (2017). Polyhydroxyalkanoate-based drug delivery systems. Polymer international, 66(5), 617-622.
Open this publication in new window or tab >>Polyhydroxyalkanoate-based drug delivery systems
2017 (English)In: Polymer international, ISSN 0959-8103, E-ISSN 1097-0126, Vol. 66, no 5, 617-622 p.Article, review/survey (Refereed) Published
Abstract [en]

Microbial polyhydroxyalkanoates (PHAs) have been a subject of significant research interest in the past few decades. The recent development of novel functionalized PHAs has opened up new possibilities to combine the good biocompatibility of PHA-based drug delivery systems to, for example, improve drug loading and release properties, targeting or imaging functionalities. This mini-review presents some recent scientific developments in the preparation of functionalized PHAs, PHA-drug and PHA-protein conjugates, multifunctional PHA nanoparticles and micelles as well as biosynthetic PHA particles for drug delivery. These developments in combination with the generally excellent biocompatibility of PHA materials are expected to further expand the interest in PHA materials for drug delivery and other therapeutic applications.

Place, publisher, year, edition, pages
WILEY, 2017
Keyword
polyhydroxyalkanoate, poly(3-hydroxybutyrate), drug delivery, nanoparticle, drug conjugate
National Category
Chemical Sciences
Identifiers
urn:nbn:se:kth:diva-206679 (URN)10.1002/pi.5282 (DOI)000398731200001 ()2-s2.0-85006314759 (Scopus ID)
Note

QC 20170510

Available from: 2017-05-10 Created: 2017-05-10 Last updated: 2017-05-10Bibliographically approved
Wu, D., Bäckström, E. & Hakkarainen, M. (2017). Starch Derived Nanosized Graphene Oxide Functionalized Bioactive Porous Starch Scaffolds. Macromolecular Bioscience, 17(6).
Open this publication in new window or tab >>Starch Derived Nanosized Graphene Oxide Functionalized Bioactive Porous Starch Scaffolds
2017 (English)In: Macromolecular Bioscience, ISSN 1616-5187, E-ISSN 1616-5195, Vol. 17, no 6Article in journal (Refereed) Published
Abstract [en]

A fully starch-derived bioactive 3D porous scaffold is developed. The bioactivity is introduced through nanosized graphene oxide (nGO) derived from starch by microwave-assisted degradation to carbon spheres and further oxidation to GO nanodots. nGO is covalently attached to starch to prepare functionalized starch (SNGO) via an esterification reaction. nGO and SNGO exhibit no cytotoxicity to MG63 at least up to 1000 µg mL−1 under (3-(4,5-Dimethylthiazol-2-yl)-2,5-diphenyltetrazolium bromide) assay. Porous scaffolds consisting of starch and SNGO (S/SNGO) or nGO (S/nGO) are prepared by freeze drying. The porosity and water uptake ability of the scaffolds depend on the concentration of nGO. Moreover, nGO, as a bioactive nanofiller, functions as an effective anchoring site for inducing CaP recrystallization in simulated body fluid. Among all modified starch-based scaffolds, the S/SNGO scaffold containing the highest concentration of covalently attached SNGO (50%) induces the largest amount of hydroxyapatite, a type of CaP crystal that is closest to bone. The prepared 3D porous nGO functionalized scaffold, thus, exhibits potential promise for bone/cartilage tissue engineering. (Figure presented.).

Place, publisher, year, edition, pages
Wiley-VCH Verlagsgesellschaft, 2017
National Category
Medical and Health Sciences Materials Engineering Polymer Technologies
Identifiers
urn:nbn:se:kth:diva-208314 (URN)10.1002/mabi.201600397 (DOI)000405565300002 ()2-s2.0-85019148208 (Scopus ID)
Note

QC 20170706

Available from: 2017-06-02 Created: 2017-06-02 Last updated: 2017-11-07Bibliographically approved
Avalos, A. S., Hakkarainen, M. & Odelius, K. (2017). Superiorly Plasticized PVC/PBSA Blends through Crotonic and Acrylic Acid Functionalization of PVC. Polymers, 9(3), Article ID 84.
Open this publication in new window or tab >>Superiorly Plasticized PVC/PBSA Blends through Crotonic and Acrylic Acid Functionalization of PVC
2017 (English)In: Polymers, ISSN 2073-4360, E-ISSN 2073-4360, Vol. 9, no 3, 84Article in journal (Refereed) Published
Abstract [en]

Superior plasticization efficiency was achieved by a grafting from functionalization of the PVC backbone. This was deduced to a synergistic effect of internal plasticization and improved intermolecular interactions between PVC and an oligomeric poly(butylene succinate-co-adipate) ( PBSA) plasticizer. A mild grafting process for functionalization of the PVC chain by crotonic acid ( CA) or acrylic acid ( AA) was used. The formation of PVC-g-CA and PVC-g-AA was confirmed by FTIR and H-1 NMR. Grafting with the seemingly similar monomers, CA and AA, resulted in different macromolecular structures. AA is easily homopolymerized and long hydrophilic poly( acrylic acid) grafts are formed resulting in branched materials. Crotonic acid does not easily homopolymerize; instead, single crotonic acid units are located along the PVC chain, leading to basically linear PVC chains with pendant crotonic acid groups. The elongation of PVC-g-CA and PVC-g-AA in comparison to pure PVC were greatly increased from 6% to 128% and 167%, respectively, by the grafting reactions. Blending 20% ( w/w) PBSA with PVC, PVC-AA or PVC-CA further increased the elongation at break to 150%, 240% and 320%, respectively, clearly showing a significant synergistic effect in the blends with functionalized PVC. This is a clearly promising milestone towards environmentally friendly flexible PVC materials.

Place, publisher, year, edition, pages
MDPI AG, 2017
Keyword
PVC, poly(butylene succinate-co-adipate), polyester, functionalization, blend, plasticizer, acrylic acid, crotonic acid
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-205519 (URN)10.3390/polym9030084 (DOI)000397231100008 ()2-s2.0-85014933563 (Scopus ID)
Note

QC 20170509

Available from: 2017-05-09 Created: 2017-05-09 Last updated: 2017-11-29Bibliographically approved
Pal, J., Wu, D., Hakkarainen, M. & Srivastava, R. K. (2017). The viscoelastic interaction between dispersed and continuous phase of PCL/HA-PVA oil-in-water emulsion uncovers the theoretical and experimental basis for fiber formation during emulsion electrospinning. European Polymer Journal, 96, 44-54.
Open this publication in new window or tab >>The viscoelastic interaction between dispersed and continuous phase of PCL/HA-PVA oil-in-water emulsion uncovers the theoretical and experimental basis for fiber formation during emulsion electrospinning
2017 (English)In: European Polymer Journal, ISSN 0014-3057, E-ISSN 1873-1945, Vol. 96, 44-54 p.Article in journal (Refereed) Published
Abstract [en]

Emulsion electrospinning was recently introduced to minimize the amount of organic solvent during electrospinning process. Here, we uncover the theoretical and experimental basis for the fiber formation in emulsion electrospinning by revealing the viscoelastic interaction between dispersed and continuous phase. Composite electrospun matrices of poly(epsilon-caprolactone) (PCL) with or without hydroxyapatite were devised from an oil-in-water emulsion. The fiber formation and uniformity were clearly governed by the viscoelastic interaction between the continuous and dispersed phase. Caging of droplets by optimal quantity of poly(vinyl alcohol) (PVA) in continuous phase resulted in uniform stretching and coalescence of droplets. An increased storage and loss modulus for emulsions containing optimum PVA manifested desired viscoelastic interaction between dispersed and continuous phase, which further resulted in uniform jet stretching. The visthelasticity of the emulsion could be tailored by changing the polymer concentration in dispersed or continuous phase, which enabled production of electrospun fibers with desired fineness.

National Category
Polymer Technologies
Identifiers
urn:nbn:se:kth:diva-218228 (URN)10.1016/j.eurpolymj.2017.09.004 (DOI)000414887700004 ()2-s2.0-85029121517 (Scopus ID)
Note

QC 20171128

Available from: 2017-11-28 Created: 2017-11-28 Last updated: 2017-11-28Bibliographically approved
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Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0002-7790-8987

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