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Conducting Polymers for Biological Studies and Medical Applications: Fabrication, Functionalisation, and Characterisation of Polypyrrole-Based Soft Actuators and Surfaces
Linköping University, Department of Physics, Chemistry and Biology, Sensor and Actuator Systems. Linköping University, Faculty of Science & Engineering.ORCID iD: 0000-0001-6333-6749
2026 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The global population is ageing rapidly, and this demographic shift, combined with sedentary lifestyles, has resulted in an increased prevalence of chronic diseases and functional impairment. Addressing these challenges requires ensuring that the increased longevity is accompanied by improved quality of life. Achieving this goal demands the development of new technologies that support mobility, rehabilitation, and health monitoring, together with a deeper understanding of fundamental cellular behaviour to enable effective therapeutic strategies. Conducting polymers (CP), e.g., polypyrrole (PPy), exhibit a unique combination of properties including electrical conductivity, tunability, biocompatibility, adaptability, and processability, making them highly attractive for a wide range of applications. In this thesis, innovative CP-based devices are explored for biological studies and medical applications, with a particular focus on soft actuators, functionalised active surfaces, and systems that combine both approaches. The work can be structured into three main parts.

The first part focuses on wearable technologies, specifically smart textile actuators based on CP-coated yarns (CP-yarns), with potential use in assistive devices. For effective integration of CP-yarns into textile-based systems, a counter-electrode-free configuration is preferred. This can be achieved by employing two yarns that actuate synchronously while undergoing opposite redox reactions. The actuation mechanism can be tuned by doping the CP-yarn with either small or large anions. Yarns doped with small, mobile anions actuate due to anion diffusion, whereas yarns doped with large, immobile anions actuate due to cation diffusion. We investigate dopants and electrolytes to obtain a complementary pair of anion- and cation-driven CP-yarns, which results in a counter-electrode-free linear actuation system. This strategy facilitates the integration of CP-based actuators into lightweight, flexible, and low-power wearable technologies for physical assistance and rehabilitation.

The second part addresses fundamental biological studies enabled by novel CP-based actuators and active surfaces. We develop a simple, versatile, PPy-coated gold (PPyAu) wire actuator for in vitro mechanotransduction studies that is compatible with cell culture conditions. The PPyAu wire actuator delivers well-controlled static and cyclic micro-mechanical stimuli to adjacent cells. Using osteoblastic and endothelial cell models, we show regime-dependent mechanotransduction responses at both transcriptional and cytoskeletal levels, e.g., upregulation of well-known mechanosensitive genes, including Fos and Fosl1, and reorganization of the cytoskeleton and maturation of focal adhesions. Altogether, these results highlight the importance of stimulation dynamics in mechanobiology. In parallel, CPs are employed as dynamic substrates for the development of advanced in vitro culture platforms. PPy surfaces functionalised with osteoblast-derived plasma membrane nanofragments (PMNFs) are engineered to promote early-stage bone mineralisation, mimicking key aspects of the bone marrow niche. We investigate the influence of PPy dopants, PPy redox state, PMNFs immobilisation strategies, mineralisation time, and the addition of β-glycerophosphate during mineralisation of the bone. Furthermore, we show that these surfaces support hematopoietic stem cells (HSCs) viability and modulate cell adhesion and proliferation, representing a promising step toward advanced biochips for in vitro studies.

Finally, the third part explores future-oriented, autonomous biohybrid systems. To date, most CP-based actuators rely on external potentiostats or wired power supplies. As an alternative, biochemical energy conversion using glucose and oxygen, as employed in enzymatic biofuel cells, offers a route toward untethered operation. To this end, we investigate the electrochemistry of enzyme-catalysed biofuel reactions in solution and on the surface in PPy-coated bilayer and trilayer bending actuators. To improve electron transfer, the use of redox mediators and enzyme immobilisation strategies are explored. This work advances the possibility of self-powered CP actuators and highlights their potential for next-generation implantable, ingestible, or wearable biomedical devices.

Overall, this thesis demonstrates how CPs can bridge device development and fundamental biological research, advancing soft actuation wearable technologies, mechanobiology tools, and autonomous biohybrid systems for future biomedical applications.

Abstract [sv]

Världens befolkning åldras snabbt och tillsammans med allt mer stillasittande livsstilar leder detta till en ökning av kroniska sjukdomar och rörelseproblem. Utmaningen är inte bara att leva längre, utan att göra det med god livskvalitet. För att uppnå detta krävs utveckling av nya teknologier som kan förbättra rörlighet och rehabilitering, samt en djupare förståelse för hur kroppens celler fungerar för att kunna utforma mer effektiva behandlingar.

Konjugerade polymerer (på engelska conducting polymers, CP) är material med en unik kombination av egenskaper. De kan leda elektricitet likt metaller, men är samtidigt flexibla, lätta, formbara och i vissa fall biokompatibla vilket är typiskt för polymerer. Dessa material finns inte naturligt utan måste syntetiseras i laboratoriet från sin utgångsmolekyl, som kallas monomer. När dessa monomerer kopplas samman bildas långa kedjor, så kallade polymerer, vars egenskaper kan anpassas efter den avsedda tillämpningen. Dessutom kan materialets egenskaper ändras efter syntesen genom att applicera en elektrisk ström. Om strömmen vänds kan materialet återgå till sitt ursprungliga tillstånd, vilket gör det möjligt att skapa dynamiska och programmerbara material.

Alla dessa egenskaper gör CP till mycket mångsidiga material med ett brett spektrum av tillämpningar. I denna avhandling har CP använts för att utveckla mjuka aktuatorer (soft actuators) och dynamiska ytor för medicinska tillämpningar och studier av cellbeteende.

Mjuka aktuatorer är enheter som genererar rörelse när de utsätts för en stimulans (elektrisk, ljusbaserad, termisk etc.). Deras funktion påminner om musklernas. När vi till exempel vill röra en arm skickar hjärnan en signal som gör att muskelfibrerna drar ihop sig eller sträcks ut. När detta sker samordnat i många muskelfibrer samtidigt uppstår rörelsen i hela armen. Av denna anledning kallas dessa mjuka aktuatorer ibland för artificiella muskler.

I den första studien användes CP för att belägga trådar som senare kan användas för att tillverka textilier. Eftersom trådarna är täckta av detta material kan de sättas i rörelse genom att applicera en elektrisk ström. När tråden integreras i ett textilmaterial förstärks rörelsen, på ett liknande sätt som i muskler. Dessa artificiella muskler, bestående av CP och textilier, kan vara intressanta som framtida material för att utveckla ergonomiska exoskelett som är betydligt mer bekväma och anpassningsbara än de som finns idag.

Vissa CP är också biokompatibla, vilket innebär att de inte orsakar avstötning eller förändrar biologiska system när de kommer i kontakt med dem. Därför kan CP även användas för att studera cellbeteende in vitro.

I den andra studien användes CP för att belägga små nålar som när de placeras intill celler och en elektrisk ström appliceras, expanderar och trycker mot cellerna på ett sätt som liknar det som sker i deras naturliga miljö. På så sätt kan cellernas respons på mekaniska stimuli studeras på ett kontrollerat sätt. Att förstå hur celler uppfattar dessa mekaniska signaler är avgörande för att förstå cellulära biologiska mekanismer och för att utveckla nya terapeutiska strategier mot sjukdomar som osteoporos eller cancer.

I andra fall är cellernas naturliga miljö mycket komplex, och därför behöver man utveckla system som kan efterlikna vissa egenskaper hos cellernas nisch. Ett sådant komplext system är benmärgen, ett mikromiljö inne i benen där stamceller finns – mycket speciella celler från vilka alla andra celltyper i kroppen kan bildas.

I den tredje studien användes CP för att skapa ytor som kan inducera benbildning in vitro med olika densiteter och därmed efterlikna mikromiljön i benmärgen. Dessa ytor kan därefter användas för att studera proliferation och differentieringsförmåga hos stamceller som odlas på dem.

Slutligen har dessa material också potential för utveckling av implanterbara medicintekniska enheter. För att CP ska kunna fungera inne i kroppen måste dock den elektriska stimulansen genereras utan kablar. Ett sätt att uppnå detta är, återigen, att efterlikna musklernas energisystem, som använder sockerarter som glukos och syre i blodet för att producera energi.

I det sista studien undersöktes därför potentialen hos CP som material i implanterbara enheter som kan generera rörelse från glukos och syre genom bioelektrokemiska reaktioner. Detta skulle göra det möjligt att utveckla aktuatorer som kan fungera inne i kroppen utan behov av batterier eller kablar.

Abstract [es]

La población mundial envejece rápidamente y, junto con estilos de vida cada vez más sedentarios, esto está provocando un aumento de enfermedades crónicas y problemas de movilidad. El reto no es solo vivir más años, sino vivirlos con buena calidad de vida. Para lograrlo, es necesario desarrollar nuevas tecnologías que ayuden a mejorar la movilidad y estrategias de rehabilitación, así como a comprender mejor el funcionamiento de las células de nuestro cuerpo para diseñar tratamientos más eficaces.

Los polímeros conjugados (del inglés conducting polymers, CP) son materiales con características únicas. Conducen la electricidad, como los metales, pero también son flexibles, ligeros, procesables y, en algunos casos, biocompatibles, como el resto de los polímeros. Estos materiales no existen en la naturaleza y deben ser sintetizados en el laboratorio a partir de su precursor, al que llamamos monómero. Al encadenar estos monómeros se crean largas cadenas, denominadas polímeros, cuyas propiedades pueden ajustarse a la futura aplicación del material. Además, una vez sintetizado, esas propiedades pueden nuevamente modificarse al aplicar una corriente eléctrica. Si se revierte dicha corriente, el material vuelve a su estado original, lo que permite crear materiales dinámicos y programables.

Todas estas características hacen de los CPs unos materiales excepcionales, con una gran variedad de aplicaciones. En esta tesis, los CPs se han empleado para desarrollar actuadores blandos (soft actuators) y superficies dinámicas para aplicaciones médicas y estudios celulares.

Los actuadores blandos son dispositivos que, al aplicarles un estímulo (eléctrico, lumínico, térmico, etc.) generan movimiento. Su funcionamiento recuerda al de los músculos: cuando queremos mover un brazo, por ejemplo, el cerebro envía una señal y las fibras musculares se contraen o se extienden. Cuando esto ocurre de manera coordinada en muchas fibras musculares al mismo tiempo, se genera el movimiento del brazo entero. Por esta razón, a estos actuadores blandos también se les denomina músculos artificiales.

En el primer estudio utilizamos CPs para recubrir hilos que posteriormente pueden emplearse para fabricar textiles. Como los hilos están cubiertos por este material, al aplicarles una corriente eléctrica, podemos hacer que se muevan. Cuando el hilo está integrado en un textil, este movimiento se amplifica, de forma similar a lo que ocurre con los músculos. Estos músculos artificiales, hechos de CPs y textiles, podrían ser interesantes como futuros materiales para desarrollar exoesqueletos ergonómicos, mucho más cómodos y adaptables que los disponibles actualmente.

Algunos CPs también son biocompatibles, es decir, al ponerse en contacto con sistemas biológicos, no generan su rechazo o alteran su comportamiento biológico. Por tanto, los CPs también pueden utilizarse para estudiar el comportamiento celular in vitro.

En el segundo estudio, los CPs se usaron para recubrir pequeñas agujas que, al colocarse adyacentes a células y aplicar una corriente eléctrica, el CP se expande y empuja las células, imitando las fuerzas que perciben en su entorno natural. De esta manera, podemos estudiar de forma controlada las respuestas celulares a los estímulos mecánicos. Entender cómo las células perciben estos estímulos mecánicos es fundamental para comprender los mecanismos biológicos celulares y desarrollar nuevas estrategias terapéuticas para enfermedades como la osteoporosis o el cáncer.

En otros casos, el entorno natural de las células es muy complejo, por lo que es necesario diseñar dispositivos que reproduzcan ciertas características del nicho celular. Uno de estos complejos entornos es la médula ósea, un microambiente situado en el interior de los huesos donde residen las células madre, células muy especiales a partir de las cuales se generan el resto de las células de nuestro cuerpo.

En el tercer estudio, los CPs se usaron para crear superficies capaces de inducir la formación de hueso in vitro con diferentes densidades, imitando así el microentorno de la médula ósea. Posteriormente, estas superficies se usaron para estudiar la proliferación y capacidad de diferenciarse de las células madre cultivadas sobre ellas.

Por último, estos materiales también tienen potencial para el desarrollo de dispositivos implantables. Sin embargo, para que los CPs puedan funcionar dentro del cuerpo, es necesario que el estímulo eléctrico se genere sin necesidad de cables. Una forma de hacerlo es, de nuevo, imitando a los músculos, que utilizan azúcares, como la glucosa, y el oxígeno en sangre para generar energía.

Finalmente, se exploró el potencial de los CPs como materiales para dispositivos implantables capaces de generar movimiento a partir de glucosa y oxígeno mediante reacciones bioelectroquímicas, lo que permitiría diseñar actuadores que funcionen dentro del cuerpo sin necesidad de baterías o cables.

Place, publisher, year, edition, pages
Linköping: Linköping University Electronic Press, 2026. , p. 110
Series
Linköping Studies in Science and Technology. Dissertations, ISSN 0345-7524 ; 2499
Keywords [en]
Conducting polymers, Polypyrrole, Soft actuators, Smart textiles, Mechanotransduction, Active cell culture systems, Untethered actuators
National Category
Textile, Rubber and Polymeric Materials
Identifiers
URN: urn:nbn:se:liu:diva-222082DOI: 10.3384/9789181184068ISBN: 9789181184051 (print)ISBN: 9789181184068 (electronic)OAI: oai:DiVA.org:liu-222082DiVA, id: diva2:2047440
Public defence
2026-04-17, Planck, F-building, Campus Valla, Linköping, 13:00 (English)
Opponent
Supervisors
Note

2026-03-20: DOI has been corrected in the E-version.

Available from: 2026-03-20 Created: 2026-03-20 Last updated: 2026-03-20Bibliographically approved
List of papers
1. Synchronous Cation-Driven and Anion-Driven Polypyrrole-Based Yarns toward In-Air Linear Actuators
Open this publication in new window or tab >>Synchronous Cation-Driven and Anion-Driven Polypyrrole-Based Yarns toward In-Air Linear Actuators
2024 (English)In: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 36, no 19, p. 9391-9405Article in journal (Refereed) Published
Abstract [en]

Conducting polymers (CP) have shown great features in building textile actuators. To date, most of the yarn-based or CP-yarn actuators have been operated in liquid electrolytes in a three-electrode-cell configuration, comprising an external counter and a reference electrode. For integration in textiles, a two-electrode system is needed, where both electrodes are in a yarn format. This can be achieved by having two CP-yarns, where one acts as the anode and the other as the cathode. For these two CP-yarns to operate synchronically, they both need to expand (or contract) during opposite reactions. This can be achieved by doping one CP-yarn with mobile anions that will expand during oxidation, while the other CP-yarn should be doped with immobile anions expanding during reduction. As a result, the same movement is created upon opposite redox reactions, both collaborating with the actuation in the same direction without the need for an external passive electrode to close the electrical circuit, which could oppose or hinder the movement. Most of the studies on textile actuators are based on cation-driven CP-yarn actuators, while little is known about anion-driven systems in CP-yarn actuators. Here, we first present a study of the effect of the dopants, solvents, and polymer layer combinations on the mechanism and strain of CP-yarns. The CP-yarns are coated with two layers: an inner poly(3,4-ethylenedioxythiophene) (PEDOT) layer and the outer and active polypyrrole (PPy) layer. According to our results, the dopant of the inner PEDOT layer seems to affect the actuation mechanism of the outer PPy layer and, thereby, of the whole CP-yarn actuator, influencing the direction of the movement and enhancing or hindering the total strain of the actuator. We show that a CP-yarn coated with PEDOT(Tos)/PPy(ClO4) and actuated in LiClO4 aqueous solution showed a pure anion-driven actuation. Next, based on the latter results, we demonstrate for the first time the dual actuation of two CP-yarns, doped with two different dopants, ClO4- and DBS-, actuating simultaneously driven by opposite redox reactions and exhibiting an average of 0.5% of strain, an important step toward in-air actuating yarns.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC, 2024
National Category
Materials Chemistry
Identifiers
urn:nbn:se:liu:diva-208455 (URN)10.1021/acs.chemmater.4c00873 (DOI)001325633800001 ()
Note

Funding Agencies|Swedish Research Council VR [2019-0368]; Promobilia Foundation [A22122]; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University [2009 00971]; Erling-Persson Family Foundation [2020-0054]; European Union [825232]

Available from: 2024-10-14 Created: 2024-10-14 Last updated: 2026-03-20
2. PPy‐Coated Wire Actuators for the Micromechanostimulation of Cells: Fabrication and Characterization
Open this publication in new window or tab >>PPy‐Coated Wire Actuators for the Micromechanostimulation of Cells: Fabrication and Characterization
Show others...
2026 (English)In: Small Science, E-ISSN 2688-4046, Vol. 6, no 3, article id e202500639Article in journal (Refereed) Published
Abstract [en]

Cellular mechanotransduction signals play a crucial role in physiological and pathological conditions, including skeletal disorders. Although various systems exist to mechanically stimulate cultured cells, most are constrained by incubator incompatibility, limited physiological relevance, nonuniform stimulation, or complexity. The objective of this article is to develop and validate a compact, incubator-compatible tool capable of delivering localized and physiologically relevant mechanical stimulation to small cell populations. Here, we introduce a polypyrrole-based wire-shaped microactuator designed to induce localized mechanical stress to adjacent cells. These wire-shaped microactuators are biocompatible, easy-to-use, and compact for use within standard in vitro cell culture systems. Using a noncontact optical method, we characterize the actuation of polypyrrole-coated wires in an aqueous NaDBS electrolyte, showing radial expansion of 1.5–8 µm depending on the deposited polypyrrole film thickness, comparable to cellular dimensions. Next, the actuation is confirmed to be robust and stable to use in cell culture media at physiological temperature. To evaluate biological relevance, osteoblastic KUSA-A1 cells are mechanically stimulated inside the incubator and transcriptomic changes are assessed. Mechanical stimulation resulted in upregulation of genes previously associated with mechanotransduction, including Fos and Fosb. Additionally, several uncharacterized long noncoding RNAs are differentially expressed, suggesting potential novel players in the mechanotransduction pathway.

Place, publisher, year, edition, pages
John Wiley & Sons, 2026
Keywords
Conducting polymers, Mechanotransduction, Osteoblasts, Polypyrrole, RNA sequencing, Soft-microactuators
National Category
Textile, Rubber and Polymeric Materials
Identifiers
urn:nbn:se:liu:diva-222081 (URN)10.1002/smsc.202500639 (DOI)001732144900030 ()2-s2.0-105032558060 (Scopus ID)
Note

Funding: This work was supported by the Japan Society for the Promotion of Science (JP23KK0163, JPJSBP120209923); Swedish Foundation for International Cooperation in Research and Higher Education (MG2019−8171); Vetenskapsrådet (VR2019−0368); Linköpings Universitet (SFO-Mat-LiU No. 2009 00971).

Available from: 2026-03-20 Created: 2026-03-20 Last updated: 2026-04-14Bibliographically approved

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Amaia Beatriz, Ortega Santos

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