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Françon, H., Wang, Z., Marais, A., Mystek, K., Piper, A., Granberg, H., . . . Wågberg, L. (2020). Ambient-Dried, 3D-Printable and Electrically Conducting Cellulose Nanofiber Aerogels by Inclusion of Functional Polymers. Advanced Functional Materials, Article ID 1909383.
Open this publication in new window or tab >>Ambient-Dried, 3D-Printable and Electrically Conducting Cellulose Nanofiber Aerogels by Inclusion of Functional Polymers
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2020 (English)In: Advanced Functional Materials, ISSN 1616-301X, E-ISSN 1616-3028, article id 1909383Article in journal (Refereed) Published
Abstract [en]

This study presents a novel, green, and efficient way of preparing crosslinked aerogels from cellulose nanofibers (CNFs) and alginate using non-covalent chemistry. This new process can ultimately facilitate the fast, continuous, and large-scale production of porous, light-weight materials as it does not require freeze-drying, supercritical CO2 drying, or any environmentally harmful crosslinking chemistries. The reported preparation procedure relies solely on the successive freezing, solvent-exchange, and ambient drying of composite CNF-alginate gels. The presented findings suggest that a highly-porous structure can be preserved throughout the process by simply controlling the ionic strength of the gel. Aerogels with tunable densities (23–38 kg m−3) and compressive moduli (97–275 kPa) can be prepared by using different CNF concentrations. These low-density networks have a unique combination of formability (using molding or 3D-printing) and wet-stability (when ion exchanged to calcium ions). To demonstrate their use in advanced wet applications, the printed aerogels are functionalized with very high loadings of conducting poly(3,4-ethylenedioxythiophene):tosylate (PEDOT:TOS) polymer by using a novel in situ polymerization approach. In-depth material characterization reveals that these aerogels have the potential to be used in not only energy storage applications (specific capacitance of 78 F g−1), but also as mechanical-strain and humidity sensors. © 2020 The Authors. 

Place, publisher, year, edition, pages
Wiley-VCH Verlag, 2020
Keywords
aerogels, cellulose, nanofibers, organic electronics, poly(3, 4-ethylenedioxythiophene), Crosslinking, Drying, Ion exchange, Ionic strength, Ions, Nanocellulose, Scales (weighing instruments), Sulfur compounds, Crosslinking chemistry, Energy storage applications, In-situ polymerization, Large scale productions, Material characterizations, Poly-3, 4-ethylenedioxythiophene, Preparation procedures, 3D printers
National Category
Natural Sciences
Identifiers
urn:nbn:se:ri:diva-43949 (URN)10.1002/adfm.201909383 (DOI)2-s2.0-85078930679 (Scopus ID)
Available from: 2020-02-19 Created: 2020-02-19 Last updated: 2020-02-19Bibliographically approved
Méhes, G., Vagin, M., Mulla, M., Granberg, H., Che, C., Beni, V., . . . Simon, D. (2020). Solar Heat-Enhanced Energy Conversion in Devices Based on Photosynthetic Membranes and PEDOT:PSS-Nanocellulose Electrodes. Advanced Sustainable Systems, 4(1), Article ID 1900100.
Open this publication in new window or tab >>Solar Heat-Enhanced Energy Conversion in Devices Based on Photosynthetic Membranes and PEDOT:PSS-Nanocellulose Electrodes
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2020 (English)In: Advanced Sustainable Systems, ISSN 2366-7486, Vol. 4, no 1, article id 1900100Article in journal (Refereed) Published
Abstract [en]

Energy harvesting from photosynthetic membranes, proteins, or bacteria through bio-photovoltaic or bio-electrochemical approaches has been proposed as a new route to clean energy. A major shortcoming of these and solar cell technologies is the underutilization of solar irradiation wavelengths in the IR region, especially those in the far IR region. Here, a biohybrid energy-harvesting device is demonstrated that exploits IR radiation, via convection and thermoelectric effects, to improve the resulting energy conversion performance. A composite of nanocellulose and the conducting polymer system poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) is used as the anode in biohybrid cells that includes thylakoid membranes (TMs) and redox mediators (RMs) in solution. By irradiating the conducting polymer electrode by an IR light-emitting diode, a sixfold enhancement in the harvested bio-photovoltaic power is achieved, without compromising stability of operation. Investigation of the output currents reveals that IR irradiation generates convective heat transfer in the electrolyte bulk, which enhances the redox reactions of RMs at the anode by suppressing diffusion limitations. In addition, a fast-transient thermoelectric component, originating from the PEDOT:PSS-nanocellulose-electrolyte interphase, further increases the bio-photocurrent. These results pave the way for the development of energy-harvesting biohybrids that make use of heat, via IR absorption, to enhance energy conversion efficiency. 

Place, publisher, year, edition, pages
Wiley-VCH Verlag, 2020
Keywords
bio-photoelectrochemical cells, bio-photovoltaic cells, energy harvesting, infrared, nanocellulose, PEDOT:PSS, thylakoid membranes
National Category
Natural Sciences
Identifiers
urn:nbn:se:ri:diva-43361 (URN)10.1002/adsu.201900100 (DOI)2-s2.0-85077874472 (Scopus ID)
Note

Funding details: 2017-03121; Funding details: Stiftelsen för Strategisk Forskning, SSF; Funding details: Knut och Alice Wallenbergs Stiftelse; Funding text 1: Major funding for this project was provided by the Knut and Alice Wallenberg Foundation and the Swedish Foundation for Strategic Research. Additional funding was provided by the ?nnesj? Foundation and the Research Institutes of Sweden (project: Bio-based electronics). G.M. was also supported by a grant from the Swedish MSCA Seal of Excellence program. G.M. was also supported by a grant from the Swedish MSCA Seal of Excellence program (Vinnova grant 2017-03121). The authors wish to thank Prof. Hans-Erik ?kerlund for advice on extraction of TMs; Dr. Jesper Edberg and Dr. Zia Ullah Khan for advice on PEDOT:PSS-CNF and PEDOT:PSS films; Dr. Pawel Wojcik for providing electrochemical setups for testing and related advice; Dr. Robert Brooke for providing GL/ITO substrates; Gustav Knutsson, Dr. Daniel Tordera, and Dr. Francesco Milano for providing experimental help and/or advice regarding excitation and heat sources; Thor Balkhed for help with video editing; and Dr. Eliot Gomez, Dr. Iwona Bernacka-Wojcik, Assoc. Prof. Magnus Jonsson, and Johannes Gladisch for fruitful discussions.

Available from: 2020-01-29 Created: 2020-01-29 Last updated: 2020-01-29Bibliographically approved
Han, S., Alvi, N. U., Granlöf, L., Granberg, H., Berggren, M., Fabiano, S. & Crispin, X. (2019). A Multiparameter Pressure–Temperature–Humidity Sensor Based on Mixed Ionic–Electronic Cellulose Aerogels. Advanced Science, Article ID 1802128.
Open this publication in new window or tab >>A Multiparameter Pressure–Temperature–Humidity Sensor Based on Mixed Ionic–Electronic Cellulose Aerogels
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2019 (English)In: Advanced Science, ISSN 2198-3844, article id 1802128Article in journal (Refereed) Published
Abstract [en]

Pressure (P), temperature (T), and humidity (H) are physical key parameters of great relevance for various applications such as in distributed diagnostics, robotics, electronic skins, functional clothing, and many other Internet-of-Things (IoT) solutions. Previous studies on monitoring and recording these three parameters have focused on the integration of three individual single-parameter sensors into an electronic circuit, also comprising dedicated sense amplifiers, signal processing, and communication interfaces. To limit complexity in, e.g., multifunctional IoT systems, and thus reducing the manufacturing costs of such sensing/communication outposts, it is desirable to achieve one single-sensor device that simultaneously or consecutively measures P–T–H without cross-talks in the sensing functionality. Herein, a novel organic mixed ion–electron conducting aerogel is reported, which can sense P–T–H with minimal cross-talk between the measured parameters. The exclusive read-out of the three individual parameters is performed electronically in one single device configuration and is enabled by the use of a novel strategy that combines electronic and ionic Seebeck effect along with mixed ion–electron conduction in an elastic aerogel. The findings promise for multipurpose IoT technology with reduced complexity and production costs, features that are highly anticipated in distributed diagnostics, monitoring, safety, and security applications. © 2019 The Authors.

Keywords
Pressure, temperature, humdity, sensor, cellulose, aerogel, Internet of Things
National Category
Electrical Engineering, Electronic Engineering, Information Engineering
Identifiers
urn:nbn:se:ri:diva-37838 (URN)10.1002/advs.201802128 (DOI)2-s2.0-85061242830 (Scopus ID)
Available from: 2019-02-28 Created: 2019-02-28 Last updated: 2019-03-05Bibliographically approved
Wang, X., Grimoldi, A., Håkansson, K., Fall, A., Granberg, H., Mengistie, D., . . . Gustafsson, G. (2019). Anisotropic conductivity of Cellulose-PEDOT:PSS composite materials studied with a generic 3D four-point probe tool. Organic electronics, 66, 258-264
Open this publication in new window or tab >>Anisotropic conductivity of Cellulose-PEDOT:PSS composite materials studied with a generic 3D four-point probe tool
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2019 (English)In: Organic electronics, ISSN 1566-1199, E-ISSN 1878-5530, Vol. 66, p. 258-264Article in journal (Refereed) Published
Abstract [en]

The conductive polymer poly(3,4-ethylenedioxythiphene):poly(styrenesulfonate) (PEDOT:PSS) is widely used in organic electronics and printed electronics due to its excellent electronic and ionic conductivity. PEDOT:PSS films exhibit anisotropic conductivities originating from the interplay of film deposition processes and chemical structure. The previous studies found that high boiling point solvent treated PEDOT:PSS exhibits an anisotropy of 3–4 orders magnitude. Even though both the in-plane and out-of-plane conductivities are important for the device performance, the out-of-plane conductivity is rarely studied due to the complexity with the experiment procedure. Cellulose-based paper or films can also exhibit anisotropic behavior due to the combination of their intrinsic fibric structure and film formation process. We have previously developed a conductive paper based on PEDOT:PSS and cellulose which could be used as the electrodes in energy storage devices. In this work we developed a novel measurement set-up for studying the anisotropy of the charge transport in such composite materials. A tool with two parallel plates mounted with spring loaded probes was constructed enabling probing both lateral and vertical directions and resistances from in-plane and out-of-plane directions to be obtained. The measurement results were then input and analyzed with a model based on a transformation method developed by Montgomery, and thus the in-plane and out-of-plane conductivities could be detangled and derived. We also investigated how the conductivity anisotropy depends on the microstructure of the cellulose template onto which the conductive polymer self-organizes. We show that there is a relatively small difference between the in-plane and out-of-plane conductivities which is attributed to the unique 3D-structure of the composites. This new knowledge gives a better understanding of the possibilities and limitations for using the material in electronic and electrochemical devices.

Keywords
Cellulose, PEDOT:PSS, Composite material, Anisotropic conductivity, Four-point probe
National Category
Natural Sciences
Identifiers
urn:nbn:se:ri:diva-36990 (URN)10.1016/j.orgel.2018.12.023 (DOI)2-s2.0-85060026237 (Scopus ID)
Available from: 2019-01-08 Created: 2019-01-08 Last updated: 2020-02-03Bibliographically approved
Erlandsson, J., Françon, H., Marais, A., Granberg, H. & Wågberg, L. (2019). Cross-Linked and Shapeable Porous 3D Substrates from Freeze-Linked Cellulose Nanofibrils.. Biomacromolecules, 20(2), 728-737
Open this publication in new window or tab >>Cross-Linked and Shapeable Porous 3D Substrates from Freeze-Linked Cellulose Nanofibrils.
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2019 (English)In: Biomacromolecules, ISSN 1525-7797, E-ISSN 1526-4602, Vol. 20, no 2, p. 728-737Article in journal (Refereed) Published
Abstract [en]

Chemically cross-linked highly porous nanocellulose aerogels with complex shapes have been prepared using a freeze-linking procedure that avoids common post activation of cross-linking reactions and freeze-drying. The aerogel shapes ranged from simple geometrical three-dimensional bodies to swirls and solenoids. This was achieved by molding or extruding a periodate oxidized cellulose nanofibril (CNF) dispersion prior to chemical cross-linking in a regular freezer or by reshaping an already prepared aerogel by plasticizing the structure in water followed by reshaping and locking the aerogel into its new shape. The new shapes were most likely retained by new cross-links formed between CNFs brought into contact by the deformation during reshaping. This self-healing ability to form new bonds after plasticization and redrying also contributed to the mechanical resilience of the aerogels, allowing them to be cyclically deformed in the dry state, reswollen with water, and redried with good retention of mechanical integrity. Furthermore, by exploiting the shapeability and available inner structure of the aerogels, a solenoid-shaped aerogel with all surfaces coated with a thin film of conducting polypyrrole was able to produce a magnetic field inside the solenoid, demonstrating electromagnetic properties. Furthermore, by biomimicking the porous interior and stiff exterior of the beak of a toucan bird, a functionalized aerogel was created by applying a 300 μm thick stiff wax coating on its molded external surfaces. This composite material displayed a 10-times higher elastic modulus compared to that of the plain aerogel without drastically increasing the density. These examples show that it is possible to combine advanced shaping with functionalization of both the inner structure and the surface of the aerogels, radically extending the possible use of CNF aerogels.

National Category
Natural Sciences
Identifiers
urn:nbn:se:ri:diva-36386 (URN)10.1021/acs.biomac.8b01412 (DOI)30394086 (PubMedID)2-s2.0-85057560598 (Scopus ID)
Available from: 2018-11-22 Created: 2018-11-22 Last updated: 2019-05-10Bibliographically approved
Granberg, H., Håkansson, K., Fall, A. & Wågberg, P. (2019). Electroactive papers, films, filaments, aerogels and hydrogels to realize the future of bio-based electronics. In: PaperCon 2019: Proceedings. Paper presented at PaperCon 2019, held in Indianapolis, Indiana, USA, 5-8 May 2019. TAPPI Press, Article ID PF4.1.
Open this publication in new window or tab >>Electroactive papers, films, filaments, aerogels and hydrogels to realize the future of bio-based electronics
2019 (English)In: PaperCon 2019: Proceedings, TAPPI Press, 2019, article id PF4.1Conference paper, Published paper (Other academic)
Abstract [en]

Research has been undertaken into the mixing of electroactive additives (EAA), for example, conducting polymers or particles, in five different cellulose structures and their further processing into electroactive papers and films. The cellulose structures considered included cellulose nanofibrils (CNF) hydrogels, CNG aerogels, CNF filaments, CNF films and cellulose papers. It has been demonstrated that the cellulose structure in combination with the electroactive polymer or particle, could be used to tailor numerous different properties. The cellulose could provide properties that support structural integrity, processability, ionic conductivity, shapeability and a large inner capacitive surface. The highly porous aerogel particles could be shaped using three-dimensional printed templates prior to freezing. The particles could be filled either with active material from the start before freeze-linking or filled with active material afterwards based on the layer by layer method. Electroactive paper could also be produced by adding the active component directly as a filler during papermaking, by adding CNF spun EA filaments cut into conveniently long staple fibres.

Place, publisher, year, edition, pages
TAPPI Press, 2019
Keywords
speciality paper, nanocellulose, aerogel, hydrogel, electrokinetics, biocompatibility, process analysis
National Category
Paper, Pulp and Fiber Technology
Identifiers
urn:nbn:se:ri:diva-43249 (URN)
Conference
PaperCon 2019, held in Indianapolis, Indiana, USA, 5-8 May 2019
Available from: 2020-01-15 Created: 2020-01-15 Last updated: 2020-01-20Bibliographically approved
Edberg, J., Brooke, R., Granberg, H., Engquist, I. & Berggren, M. (2019). Improving the Performance of Paper Supercapacitors Using Redox Molecules from Plants. Advanced Sustainable Systems, 3(8), Article ID 1900050.
Open this publication in new window or tab >>Improving the Performance of Paper Supercapacitors Using Redox Molecules from Plants
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2019 (English)In: Advanced Sustainable Systems, Vol. 3, no 8, article id 1900050Article in journal (Refereed) Published
Abstract [en]

A supercapacitor made from organic and nature‐based materials, such as conductive polymers (PEDOT:PSS), nanocellulose, and an the organic dye molecule (alizarin), is demonstrated. The dye molecule, which historically was extracted from the roots of the plant rubia tinctorum, is here responsible for the improvement in energy storage capacity, while the conductive polymer provides bulk charge transport within the composite electrode. The forest‐based nanocellulose component provides a mechanically strong and nonporous network onto which the conductive polymer self‐organizes. The electrical and electrochemical properties of the material composition are investigated and prototype redox‐enhanced supercapacitor devices with excellent specific capacitance exceeding 400 F g−1 and an operational stability over >1000 cycles are demonstrated. This new class of supercapacitors, which in part are based on organic materials from plants, represents an important step toward a green and sustainable energy technology.

National Category
Natural Sciences
Identifiers
urn:nbn:se:ri:diva-39696 (URN)10.1002/adsu.201900050 (DOI)2-s2.0-85070784704 (Scopus ID)
Available from: 2019-08-08 Created: 2019-08-08 Last updated: 2020-01-10Bibliographically approved
Granberg, H., Sandberg, M. & Håkansson, K. (2019). Pilot scale production of interactive zinc oxide paper and its multiple applicability. In: PaperCon 2019: Proceedings. Paper presented at PaperCon 2019. Proceedings of a conference held in Indianapolis, Indiana, USA, 5-8 May 2019. TAPPI Press, Article ID PF3.3.
Open this publication in new window or tab >>Pilot scale production of interactive zinc oxide paper and its multiple applicability
2019 (English)In: PaperCon 2019: Proceedings, TAPPI Press, 2019, article id PF3.3Conference paper, Published paper (Other academic)
Abstract [en]

A study has been made of the production of zinc oxide (ZnO) paper in a pilot paper machine. Bleached sulphate softwood pulp (70%) and bleached sulphate hardwood pulp (30%) were corefined. Cationic polyacrylamide (CPAM) was used as retention agent, while alkyl ketene dimer (AKD) was used as sizing agent for some samples. Some papers were screen printed with a conducting carbon-based ink to produce a photosensor device. Two methods were used to study the photocatalysis: immersing ZnO papers into kongo red dispersions or resazurin (Rz) based photocatalyst activity indicator ink and exposing the papers to ultraviolet (UV) light in a sunlight simulator. ZnO papers of approximately 60gsm were successfully produced on the pilot scale machine, which was run at a low speed (100m/min) and the retention of ZnO particles was good in all samples. The paper looked like an ordinary white printing paper product, but was a truly interactive material, exhibiting photoconductivity and enabling use as an excellent photosensor.

Place, publisher, year, edition, pages
TAPPI Press, 2019
Keywords
speciality paper, zinc oxide, pilot trial, paper properties, photoconductivity, photoconductor
National Category
Paper, Pulp and Fiber Technology
Identifiers
urn:nbn:se:ri:diva-40586 (URN)
Conference
PaperCon 2019. Proceedings of a conference held in Indianapolis, Indiana, USA, 5-8 May 2019
Available from: 2019-10-28 Created: 2019-10-28 Last updated: 2019-10-31Bibliographically approved
Erlandsson, J., Pettersson, T., Ingverud, T., Granberg, H., Larsson, P. A., Malkoch, M. & Wågberg, L. (2018). On the mechanism behind freezing-induced chemical crosslinking in ice-templated cellulose nanofibril aerogels. Journal of Materials Chemistry A, 6(40), 19371-19380
Open this publication in new window or tab >>On the mechanism behind freezing-induced chemical crosslinking in ice-templated cellulose nanofibril aerogels
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2018 (English)In: Journal of Materials Chemistry A, ISSN 2050-7488, Vol. 6, no 40, p. 19371-19380Article in journal (Refereed) Published
Abstract [en]

The underlying mechanism related to freezing-induced crosslinking of aldehyde-containing cellulose nanofibrils (CNFs) has been investigated, and the critical parameters behind this process have been identified. The aldehydes introduced by periodate oxidation allows for formation of hemiacetal bonds between the CNFs provided the fibrils are in sufficiently close contact before the water is removed. This is achieved during the freezing process where the cellulose components are initially separated, and the growth of ice crystals forces the CNFs to come into contact in the thin lamellae between the ice crystals. The crosslinked 3-D structure of the CNFs can subsequently be dried under ambient conditions after solvent exchange and still maintain a remarkably low density of 35 kg m-3, i.e. a porosity greater than 98%. A lower critical amount of aldehydes, 0.6 mmol g-1, was found necessary in order to generate a crosslinked 3-D CNF structure of sufficient strength not to collapse during the ambient drying. The chemical stability of the 3-D structure can be further enhanced by converting the hemiacetals to acetals by treatment with an alcohol under acidic conditions.

Place, publisher, year, edition, pages
Royal Society of Chemistry, 2018
Keywords
Aerogels, Aldehydes, Cellulose, Chemical stability, Crosslinking, Freezing, Nanofibers
National Category
Paper, Pulp and Fiber Technology Nano Technology
Identifiers
urn:nbn:se:ri:diva-35538 (URN)10.1039/c8ta06319b (DOI)2-s2.0-85055128762 (Scopus ID)
Funder
Swedish Energy Agency
Note

cited By 0

Available from: 2018-10-30 Created: 2018-10-30 Last updated: 2018-10-30Bibliographically approved
Edberg, J., Malti, A., Granberg, H., Hamedi, M. M., Crispin, X., Engquist, I. & Berggren, M. (2017). Electrochemical circuits from ’cut and stick’ PEDOT:PSS-nanocellulose composite. Flexible and Printed Electronics, 2(4), Article ID 045010.
Open this publication in new window or tab >>Electrochemical circuits from ’cut and stick’ PEDOT:PSS-nanocellulose composite
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2017 (English)In: Flexible and Printed Electronics, Vol. 2, no 4, article id 045010Article in journal (Refereed) Published
Abstract [en]

Wereport a flexible self-standing adhesive composite made from PEDOT:PSS and nanofibrillated cellulose. The material exhibits good combined mechanical and electrical characteristics (an elastic modulus of 4.4 MPa, and an electrical conductivity of 30 S cm-1). The inherent self-adhesiveness of the material enables it to be laminated and delaminated repeatedly to form and reconfigure devices and circuits. This modular property opens the door for a plethora of applications where reconfigurability and ease-of-manufacturing are of prime importance. Wealso demonstrate a paper composite with ionic conductivity and combine the two materials to construct electrochemical devices, namely transistors, capacitors and diodes with high values of transconductance, charge storage capacity and current rectification.Wehave further used these devices to construct digital circuits such as NOT, NANDandNORlogic.

Keywords
flexible electronics, nanocellulose, organic electronics, PEDOT, supercapacitators
National Category
Nano Technology Electrical Engineering, Electronic Engineering, Information Engineering
Identifiers
urn:nbn:se:ri:diva-33328 (URN)10.1088/2058-8585/aa8027 (DOI)2-s2.0-85041011470 (Scopus ID)
Funder
Knut and Alice Wallenberg Foundation, KAW 2011.0050Swedish Foundation for Strategic Research
Note

cited By 0

Available from: 2018-02-28 Created: 2018-02-28 Last updated: 2019-01-02Bibliographically approved
Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0003-0838-3977

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