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Nanocellulose and Polypyrrole Composites for Electrical Energy Storage
Uppsala University, Disciplinary Domain of Science and Technology, Technology, Department of Engineering Sciences, Nanotechnology and Functional Materials.
2012 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

To meet the predicted increase in demand for energy storage in tomorrow's society, the development of inexpensive, flexible, lightweight and sustainable energy-storage materials is essential. In this respect, devices based on electroactive organic molecules, such as conducting polymers, are highly interesting. The aim of this thesis was to evaluate the use of nanocellulose as a matrix material in composites of cellulose and the electroactive polymer polypyrrole (PPy), and the use of these composites in all-polymer paper-based energy-storage devices.  

Pyrrole was polymerized using FeCl3 onto cellulose nanofibers in the form of a hydrogel. The resulting PPy-coated fibers were washed with water and dried into a high surface area, conductive paper material. Variations in the drying technique provided a way of controlling the porosity and the surface area of wood-based cellulose nanofibers, as the properties of the cellulose were found to have a large influence on the composite structure. Different nanocellulose fibers, of algal and wood origin, were evaluated as the reinforcing phase in the conductive composites. These materials had conductivities of 1–6 S/cm and specific surface areas of up to 246 m2/g at PPy weight fractions around 67%.  

Symmetrical supercapacitor devices with algae-based nanocellulose-PPy electrodes and an aqueous electrolyte showed specific charge capacities of around 15 mAh/g and specific capacitances of around 35 F/g, normalized with respect to the dry electrode weight. Potentiostatic charging of the devices was suggested as a way to make use of the rapid oxidation and reduction processes in these materials, thus minimizing the charging time and the effect of the IR drop in the device, and ensuring charging to the right potential. Repeated charging and discharging of the devices revealed a 10–20% loss in capacity over 10 000 cycles. Upon up-scaling of the devices, it was found that an improved cell design giving a lower cell resistance was needed in order to maintain high charge and discharge rates.  

The main advantages of the presented concept of nanocellulose-PPy-based electrical energy storage include the eco-friendly raw materials, an up-scalable and potentially cost-effective production process, safe operation, and the controllable porosity and moldability offered by the nanocellulose fiber matrix. Integrating energy storage devices into paper could lead to un- precedented opportunities for new types of consumer electronics. Future research efforts should be directed at increasing the energy density and improving the stability of this type of device as well as advancing the fundamental understanding of the current limitations of these properties.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2012. , 71 p.
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 898
Keyword [en]
conducting polymer, polypyrrole, cellulose, nanocellulose, porosity, composite, energy storage, battery, supercapacitor
National Category
Physical Sciences
Research subject
Engineering Science with specialization in Materials Science
Identifiers
URN: urn:nbn:se:uu:diva-168664ISBN: 978-91-554-8276-3 (print)OAI: oai:DiVA.org:uu-168664DiVA: diva2:502077
Public defence
2012-03-30, Häggsalen, Ångströmlaboratoriet, Lägerhyddsvägen 1, Uppsala, 09:30 (English)
Opponent
Supervisors
Available from: 2012-03-09 Created: 2012-02-14 Last updated: 2012-03-29Bibliographically approved
List of papers
1. Ultrafast All-Polymer Paper-Based Batteries
Open this publication in new window or tab >>Ultrafast All-Polymer Paper-Based Batteries
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2009 (English)In: Nano letters (Print), ISSN 1530-6984, E-ISSN 1530-6992, Vol. 9, no 10, 3635-3639 p.Article in journal (Refereed) Published
Abstract [en]

Conducting polymers for battery applications have been subject to numerous investigations during the last two decades. However, the functional charging rates and the cycling stabilities have so far been found to be insufficient for practical applications. These shortcomings can, at least partially, be explained by the fact that thick layers of the conducting polymers have been used to obtain sufficient capacities of the batteries. In the present letter, we introduce a novel nanostructured high-surface area electrode material for energy storage applications composed of cellulose fibers of algal origin individually coated with a 50 nm thin layer of polypyrrole. Our results show the hitherto highest reported charge capacities and charging rates for an all polymer paper-based battery. The composite conductive paper material is shown to have a specific surface area of 80 m(2) g(-1) and batteries based on this material can be charged with currents as high as 600 mA cm(-2) with only 6% loss in capacity over 100 subsequent charge and discharge cycles. The aqueous-based batteries, which are entirely based on cellulose and polypyrrole and exhibit charge capacities between 25 and 33 mAh g(-1) or 38-50 mAh g(-1) per weight of the active material, open up new possibilities for the production of environmentally friendly, cost efficient, up-scalable and lightweight energy storage systems.

Place, publisher, year, edition, pages
American Chemical Society, 2009
National Category
Engineering and Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-108553 (URN)10.1021/nl901852h (DOI)000270670500045 ()19739594 (PubMedID)
Available from: 2009-09-22 Created: 2009-09-22 Last updated: 2017-12-13Bibliographically approved
2. Cycling stability and self-protective properties of a paper-based polypyrrole energy storage device
Open this publication in new window or tab >>Cycling stability and self-protective properties of a paper-based polypyrrole energy storage device
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2011 (English)In: Electrochemistry communications, ISSN 1388-2481, E-ISSN 1873-1902, Vol. 13, no 8, 869-871 p.Article in journal (Refereed) Published
Abstract [en]

A composite consisting of polypyrrole and cellulose from the Cladophora sp. green algae is shown to exhibit excellent cycling stability when used as the electrodes in an aqueous symmetric supercapacitor device. The capacitance of the device, which was 32.4 F g− 1, only decreased by 0.7% during 4000 galvanostatic cycles employing a current of 10 mA and potential cut-off limits of 0 and 0.8 V. No change in the electrode material's morphology could be seen when comparing cycled and pristine materials with scanning electron microscopy. Furthermore, no significant loss in capacitance was observed even when charging the device to 1.8 V. Measurements of the electrode potentials versus a common reference show that this effect was due to a device intrinsic self-protective mechanism which prevented degradation of the polypyrrole.

Keyword
Conducting polymer, Polypyrrole, Cycling stability, Composite, Cellulose
National Category
Natural Sciences Inorganic Chemistry Engineering and Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials; Chemistry with specialization in Inorganic Chemistry
Identifiers
urn:nbn:se:uu:diva-156540 (URN)10.1016/j.elecom.2011.05.024 (DOI)000294582300032 ()
Available from: 2011-08-01 Created: 2011-08-01 Last updated: 2017-12-08Bibliographically approved
3. Rapid Potential Step Charging of Paper-based Polypyrrole Energy Storage Devices
Open this publication in new window or tab >>Rapid Potential Step Charging of Paper-based Polypyrrole Energy Storage Devices
2012 (English)In: Electrochimica Acta, ISSN 0013-4686, E-ISSN 1873-3859, Vol. 70, 91-97 p.Article in journal (Refereed) Published
Abstract [en]

Symmetric paper-based supercapacitor devices containing polypyrrole (PPy)-cellulose composite electrodes and aqueous electrolytes can be charged using either potential step or constant current charging. Potential step charging provides better control of the charging and can result in significantly shorter charging times, enabling charging in 22s for devices with cell capacitances of 12.2F when charged to 0.8 V. The paper-based electrode material was compatible with charging currents as large as 5.9 A g(-1) due to the rapid counter ion mass transport resulting from the porous composite structure and the thin PPy coatings. The charging times were controlled by the RC time constants of the devices and the cell resistance was found to decrease with increasing electrode area. For small cells, the cell resistance was determined to a large extent by the electrolyte resistance and contact resistances, whereas the resistance of the current collectors dominated for larger cells. The specific cell capacitance was 38.3 F g(-1) or 2.1 F cm(-2), normalized with respect to the total electrode weight and electrode cross section area respectively, and the devices showed 80-90% capacitance retention after 10 000 potential step charge and discharge cycles. These results, which demonstrate that potential step charging can be advantageous for conducting polymer based energy storage devices, are very encouraging for the development of new up-scalable paper-based energy storage devices.

Keyword
Conducting polymer, Polypyrrole, Cellulose, Potential step charging, Supercapacitor
National Category
Natural Sciences Nano Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-168663 (URN)10.1016/j.electacta.2012.03.060 (DOI)000304497000012 ()
Available from: 2012-02-14 Created: 2012-02-14 Last updated: 2017-12-07Bibliographically approved
4. A Nanocellulose Polypyrrole Composite Based on Microfibrillated Cellulose from Wood
Open this publication in new window or tab >>A Nanocellulose Polypyrrole Composite Based on Microfibrillated Cellulose from Wood
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2010 (English)In: Journal of Physical Chemistry B, ISSN 1520-6106, E-ISSN 1520-5207, Vol. 114, no 12, 4178-4182 p.Article in journal (Refereed) Published
Abstract [en]

It is demonstrated that it is possible to coat the individual fibers of wood-based nanocellulose with polypyrrole using in situ chemical polymerization to obtain an electrically conducting continuous high-surface-area composite. The experimental results indicate that the high surface area of the water dispersed material, to a large extent, is maintained upon normal drying without the use of any solvent exchange. Thus, the employed chemical polymerization of polypyrrole on the microfibrillated cellulose (MFC) nanofibers in the hydrogel gives rise to a composite, the structure of which—unlike that of uncoated MFC paper—does not collapse upon drying. The dry composite has a surface area of 90 m2/g and a conductivity of 1.5 S/cm, is electrochemically active, and exhibits an ion-exchange capacity for chloride ions of 289 C/g corresponding to a specific capacity of 80 mAh/g. The straightforwardness of the fabrication of the present nanocellulose composites should significantly facilitate industrial manufacturing of highly porous, electroactive conductive paper materials for applications including ion-exchange and paper-based energy storage devices.

Place, publisher, year, edition, pages
American Chemical Society, 2010
National Category
Chemical Sciences Inorganic Chemistry Engineering and Technology
Research subject
Chemistry with specialization in Inorganic Chemistry; Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-121745 (URN)10.1021/jp911272m (DOI)000275855800010 ()20205378 (PubMedID)
Available from: 2010-03-29 Created: 2010-03-29 Last updated: 2017-12-12
5. Electroactive Nanofibrillated Cellulose Aerogel Composites with Tunable Structural Properties and High Mechanical Strength
Open this publication in new window or tab >>Electroactive Nanofibrillated Cellulose Aerogel Composites with Tunable Structural Properties and High Mechanical Strength
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(English)Article in journal (Refereed) Submitted
National Category
Natural Sciences
Identifiers
urn:nbn:se:uu:diva-168662 (URN)
Available from: 2012-02-14 Created: 2012-02-14 Last updated: 2012-03-29Bibliographically approved

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