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Monopolar and Bipolar Membranes in Organic Bioelectronic Devices
Linköping University, Department of Science and Technology, Physics and Electronics. Linköping University, The Institute of Technology. (Laboratory of Organic Electronics)ORCID iD: 0000-0002-0302-226X
2014 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

In the 1970s it was discovered that organic polymers, a class of materials otherwise best know as insulating plastics, could be made electronically conductive. As an alternative to silicon semiconductors, organic polymers offer many novel features, characteristics, and opportunities, such as producing electronics at low costs using printing techniques, using organic chemistry to tune optical and electronic properties, and mechanical flexibility. The conducting organic polymers have been used in a vast array of devices, exemplified by organic transistors, light-emitting diodes, and solar cells. Due to their softness, biocompatibility, and combined electronic and ionic transport, organic electronic materials are also well suited as the active material in bioelectronic applications, a scientific and engineering area in which electronics interface with biology. The coupling of ions and electrons is especially interesting, as ions serve as signal carriers in all living organisms, thus offering a direct translation of electronic and ionic signals. To further enable complex control of ionic fluxes, organic electronic materials can be integrated with various ionic components, such as ion-conducting diodes and transistors.

This thesis reports a background to the field of organic bioelectronic and ionic devices, and also presents the integration of ionic functions into organic bioelectronic devices. First, an electrophoretic drug delivery device is presented, capable of delivering ions at high spatiotemporal resolution. The device, called the organic electronic ion pump, is used to electronically control amyloid-like aggregation kinetics and morphology of peptides, and offers an interesting method for studying amyloids in vitro. Second, various ion-conducting diodes based on bipolar membranes are described. These diodes show high rectification ratio, i.e. conduct ions better for positive than for negative applied voltage. Simple ion diode based circuits, such as an AND gate and a full-wave rectifier, are also reported. The AND gate is intended as an addressable pH pixel to regulate for example amyloid aggregation, while the full-wave rectifier decouples the electrochemical capacity of an electrode from the amount of ionic charge it can generate. Third, an ion transistor, also based on bipolar membranes, is presented. This transistor can amplify and control ionic currents, and is suitable for building complex ionic logic circuits. Together, these results provide a basic toolbox of ionic components that is suitable for building more complex and/or implantable organic bioelectronic devices.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2014. , 76 p.
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 1620
Keyword [en]
bioelectronics, ionic, ion transport;bipolar membrane, conjugated polymer, amyloid, self-assembly
National Category
Other Electrical Engineering, Electronic Engineering, Information Engineering
Identifiers
URN: urn:nbn:se:liu:diva-110406DOI: 10.3384/diss.diva-110406ISBN: 978-91-7519-244-4 (print)OAI: oai:DiVA.org:liu-110406DiVA: diva2:745472
Public defence
2014-10-10, K2, Kåkenhus, Campus Norrköping, Linköpings Universitet, Norrköping, 10:00 (English)
Opponent
Supervisors
Available from: 2014-09-10 Created: 2014-09-10 Last updated: 2017-02-03Bibliographically approved
List of papers
1. Spatially Controlled Amyloid Reactions Using Organic Electronics
Open this publication in new window or tab >>Spatially Controlled Amyloid Reactions Using Organic Electronics
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2010 (English)In: SMALL, ISSN 1613-6810, Vol. 6, no 19, 2153-2161 p.Article in journal (Refereed) Published
Abstract [en]

Abnormal protein aggregates, so called amyloid fibrils, are mainly known as pathological hallmarks of a wide range of diseases, but in addition these robust well-ordered self-assembled natural nanostructures can also be utilized for creating distinct nanomaterials for bioelectronic devices. However, current methods for producing amyloid fibrils in vitro offer no spatial control. Herein, we demonstrate a new way to produce and spatially control the assembly of amyloid-like structures using an organic electronic ion pump (OEIP) to pump distinct cations to a reservoir containing a negatively charged polypeptide. The morphology and kinetics of the created proteinaceous nanomaterials depends on the ion and current used, which we leveraged to create layers incorporating different conjugated thiophene derivatives, one fluorescent (p-FTAA) and one conducting (PEDOT-S). We anticipate that this new application for the OEIP will be useful for both biological studies of amyloid assembly and fibrillogenesis as well as for creating new bioelectronic nanomaterials and devices.

Place, publisher, year, edition, pages
John Wiley and Sons, Ltd, 2010
National Category
Engineering and Technology
Identifiers
urn:nbn:se:liu:diva-61175 (URN)10.1002/smll.201001157 (DOI)000283274100013 ()
Available from: 2010-11-08 Created: 2010-11-05 Last updated: 2017-02-03
2. Controlled Microscopic Formation of Amyloid-Like Aβ Aggregates Using an Organic Electronic Device
Open this publication in new window or tab >>Controlled Microscopic Formation of Amyloid-Like Aβ Aggregates Using an Organic Electronic Device
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(English)Manuscript (preprint) (Other academic)
Abstract [en]

Alzheimer’s disease (AD), primarily associated with formation of fibrillar amyloid-beta peptide (Aβ) aggregates in the brain, is one of the most common old-age diseases. It is therefore crucial with an elevated scientific interest in Aβ, and its fundamental properties in a wide sense, to develop efficient methods for early detection and to combat AD. For the development of new techniques, both for AD detection and prevention, researchers are dependent on either tissue samples from deceased patients, animal models or in vitro systems. In vitro systems, such as producing protein aggregates of the Aβ-peptide in a test tube by incubation under denaturing conditions, offers us a simple but rather blunt tool for evaluating aggregation inhibition caused by compounds or to investigate new detection methods. We recently introduced the organic electronic ion pump (OEIP) as a method for creating amyloid-like aggregates at high spatiotemporal control as compared to the resulting aggregates manufactured using regular test tube-conditions. Combined with a fluorescent probe that is specific for the fibrillar aggregated form of misfolded peptides commonly seen in AD, this allowed us to control and to monitor the aggregation of a model peptide system in a highly confined space.

To further elaborate the functionality of the OEIP together with amyloid-specific probes, we here present experiments demonstrating electronically controlled micron sized formation of Aβ-aggregates with morphologies ranging from fine fibers, to bundles of fibers, and thick mesh-like fiber structures. We foresee that the methodology can be implemented in multi array systems that can be utilized for studies of protein aggregation in confined spaces or together with cultured cells, as well as for the development of screening platforms for assessment of molecules influencing the Aβ-aggregation process.

National Category
Polymer Technologies Other Electrical Engineering, Electronic Engineering, Information Engineering Biochemistry and Molecular Biology
Identifiers
urn:nbn:se:liu:diva-110401 (URN)
Available from: 2014-09-10 Created: 2014-09-10 Last updated: 2017-02-03Bibliographically approved
3. Ion diode logics for pH control
Open this publication in new window or tab >>Ion diode logics for pH control
2012 (English)In: Lab on a Chip, ISSN 1473-0197, E-ISSN 1473-0189, Vol. 12, no 14, 2507-2513 p.Article in journal (Refereed) Published
Abstract [en]

Electronic control over the generation, transport, and delivery of ions is useful in order to regulate reactions, functions, and processes in various chemical and biological systems. Different kinds of ion diodes and transistors that exhibit non-linear current versus voltage characteristics have been explored to generate chemical gradients and signals. Bipolar membranes (BMs) exhibit both ion current rectification and water splitting and are thus suitable as ion diodes for the regulation of pH. To date, fast switching ion diodes have been difficult to realize due to accumulation of ions inside the device structure at forward bias – charges that take a long time to deplete at reverse bias. Water splitting occurs at elevated reverse voltage bias and is a feature that renders high ion current rectification impossible. This makes integration of ion diodes in circuits difficult. Here, we report three different designs of micro-fabricated ion bipolar membrane diodes (IBMDs). The first two designs consist of single BM configurations, and are capable of either splitting water or providing high current rectification. In the third design, water-splitting BMs and a highly-rectifying BM are connected in series, thus suppressing accumulation of ions. The resulting IBMD shows less hysteresis, faster off-switching, and also a high ion current rectification ratio as compared to the single BM devices. Further, the IBMD was integrated in a diode-based AND gate, which is capable of controlling delivery of hydroxide ions into a receiving reservoir.

Place, publisher, year, edition, pages
Cambridge, UK: Royal Society of Chemistry, 2012
National Category
Natural Sciences
Identifiers
urn:nbn:se:liu:diva-78002 (URN)10.1039/C2LC40093F (DOI)000305532600009 ()
Available from: 2012-06-04 Created: 2012-06-04 Last updated: 2017-12-07
4. Polyphosphonium-based bipolar membranes for rectification of ionic currents
Open this publication in new window or tab >>Polyphosphonium-based bipolar membranes for rectification of ionic currents
2013 (English)In: Biomicrofluidics, ISSN 1932-1058, E-ISSN 1932-1058, Vol. 7, no 6, 064117- p.Article in journal (Refereed) Published
Abstract [en]

Bipolar membranes (BMs) have interesting applications within the field of bioelectronics, as they may be used to create non-linear ionic components (e. g., ion diodes and transistors), thereby extending the functionality of, otherwise linear, electrophoretic drug delivery devices. However, BM based diodes suffer from a number of limitations, such as narrow voltage operation range and/or high hysteresis. In this work, we circumvent these problems by using a novel polyphosphonium-based BM, which is shown to exhibit improved diode characteristics. We believe that this new type of BM diode will be useful for creating complex addressable ionic circuits for delivery of charged biomolecules.

Place, publisher, year, edition, pages
American Institute of Physics (AIP), 2013
National Category
Engineering and Technology
Identifiers
urn:nbn:se:liu:diva-103883 (URN)10.1063/1.4850795 (DOI)000329292200020 ()
Available from: 2014-01-30 Created: 2014-01-30 Last updated: 2017-12-06
5. A Four-Diode Full-Wave Ionic Current Rectifier Based on Bipolar Membranes: Overcoming the Limit of Electrode Capacity
Open this publication in new window or tab >>A Four-Diode Full-Wave Ionic Current Rectifier Based on Bipolar Membranes: Overcoming the Limit of Electrode Capacity
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2014 (English)In: Advanced Materials, ISSN 0935-9648, E-ISSN 1521-4095, Vol. 26, no 30, 5143-5147 p.Article in journal (Refereed) Published
Abstract [en]

Full-wave rectification of ionic currents is obtained by constructing the typical four-diode bridge out of ion conducting bipolar membranes. Together with conjugated polymer electrodes addressed with alternating current, the bridge allows for generation of a controlled ionic direct current for extended periods of time without the production of toxic species or gas typically arising from electrode side-reactions.

Place, publisher, year, edition, pages
Wiley-VCH Verlagsgesellschaft, 2014
Keyword
bioelectronics, ionics, ion transport, bipolar membranes, conjugated polymer electrodes
National Category
Other Electrical Engineering, Electronic Engineering, Information Engineering Polymer Technologies
Identifiers
urn:nbn:se:liu:diva-110403 (URN)10.1002/adma.201401258 (DOI)000340546300010 ()24863171 (PubMedID)
Funder
Vinnova, 2010–00507EU, FP7, Seventh Framework Programme, iONE-FP7Swedish Research Council, 621–2011–3517EU, FP7, Seventh Framework Programme, OrgBIO
Available from: 2014-09-10 Created: 2014-09-10 Last updated: 2017-12-05Bibliographically approved
6. Polyphosphonium-Based Ion Bipolar Junction Transistors
Open this publication in new window or tab >>Polyphosphonium-Based Ion Bipolar Junction Transistors
2014 (English)In: Biomicrofluidics, ISSN 1932-1058, E-ISSN 1932-1058, Vol. 8, no 6, 064116- p.Article in journal (Refereed) Published
Abstract [en]

Advancements in the field of electronics during the past few decades have inspired the use of transistors in a diversity of research fields, including biology and medicine. However, signals in living organisms are not only carried by electrons, but also through fluxes of ions and biomolecules. Thus, in order to implement the transistor functionality to control biological signals, devices that can modulate currents of ions and biomolecules, i.e. ionic transistors and diodes, are needed. One successful approach for modulation of ionic currents is to use oppositely charged ion-selective membranes to form so called ion bipolar junction transistors (IBJTs). Unfortunately, overall IBJT device performance has been hindered due to the typical low mobility of ions, large geometries of the ion bipolar junction materials, and the possibility of electric field enhanced (EFE) water dissociation in the junction. Here, we introduce a novel polyphosphonium-based anion-selective material into npn-type IBJTs. The new material does not show EFE water dissociation and therefore allows for a reduction of junction length down to 2 μm, which significantly improves the switching performance of the ion transistor to 2 s. The presented improvement in speed as well the simplified design will be useful for future development of advanced iontronic circuits employing IBJTs, for example addressable drug-delivery devices.

Keyword
WATER DISSOCIATION; NANOFLUIDIC DIODE; MEMBRANES; CIRCUITS
National Category
Other Electrical Engineering, Electronic Engineering, Information Engineering
Identifiers
urn:nbn:se:liu:diva-110400 (URN)10.1063/1.4902909 (DOI)000347160400018 ()
Note

This research was financed by VINNOVA (OBOE Miljo and AFM), the Swedish Research Council, and the Onnesjo foundation.

Available from: 2014-09-10 Created: 2014-09-10 Last updated: 2017-12-05Bibliographically approved

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