| 1. |
- Diacci, Chiara, et al.
(författare)
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Real-Time Monitoring of Glucose Export from Isolated Chloroplasts Using an Organic Electrochemical Transistor
- 2020
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Ingår i: Advanced Materials Technologies. - : Wiley-VCH Verlagsgesellschaft. - 2365-709X. ; 5:3
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Tidskriftsartikel (refereegranskat)abstract
- Biosensors based on organic electrochemical transistors (OECT) are attractive devices for real-time monitoring of biological processes. The direct coupling between the channel of the OECT and the electrolyte enables intimate interfacing with biological environments at the same time bringing signal amplification and fast sensor response times. So far, these devices are mainly applied to mammalian systems; cells or body fluids for the development of diagnostics and various health status monitoring technology. Yet, no direct detection of biomolecules from cells or organelles is reported. Here, an OECT glucose sensor applied to chloroplasts, which are the plant organelles responsible for the light-to-chemical energy conversion of the photosynthesis, is reported. Real-time monitoring of glucose export from chloroplasts in two distinct metabolic phases is demonstrated and the transfer dynamics with a time resolution of 1 min is quantified, thus reaching monitoring dynamics being an order of magnitude better than conventional methods.
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| 2. |
- Dufil, Gwennael, et al.
(författare)
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Enzyme-assisted in vivo polymerisation of conjugated oligomer based conductors
- 2020
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Ingår i: Journal of materials chemistry. B. - : ROYAL SOC CHEMISTRY. - 2050-750X .- 2050-7518. ; 8:19, s. 4221-4227
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Tidskriftsartikel (refereegranskat)abstract
- Conjugated polymers conduct both electronic and ionic carriers and thus can stimulate and translate biological signals when used as active materials in bioelectronic devices. Self- and on-demand organization of the active material directly in the in vivo environment can result in the seamless integration of the bioelectronic interface. Along that line, we recently demonstrated spontaneous in vivo polymerization of the conjugated oligomer ETE-S in the vascular tissue of plants and the formation of conducting wires. In this work, we elucidate the mechanism of the in vivo polymerization of the ETE-S trimer and demonstrate that ETE-S polymerizes due to an enzymatic reaction where the enzyme peroxidase is the catalyst and hydrogen peroxide is the oxidant. ETE-S, therefore, represents the first example of a conducting polymer that is enzymatically polymerized in vivo. By reproducing the reaction in vitro, we gain further insight on the polymerization mechanism and show that hydrogen peroxide is the limiting factor. In plants the ETE-S triggers the catalytic cycle responsible for the lignification process, hacks this biochemical pathway and integrates within the plant cell wall, forming conductors along the plant structure.
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| 3. |
- Dufil, Gwennaël, 1995-
(författare)
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Living biohybrid systems via in vivo polymerization of thiophene oligomers
- 2022
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Life is the result of a multitude of electrical signals which drives our nervous system but also accomplishes a cascade of electrochemical reactions. In the 18th century, Lucia Galeazzi and Luigi Galvani got the idea to stimulate frog legs with electrodes. This first step into the world of bioelectronics showed that electronic systems were able to communicate with living organisms through electrical stimulation, as well as by recording electrical signals from organisms. Until the end of the 20th century, the field of bioelectronics kept progressing using metal electrodes. This class of material inherently exhibits a high conductivity from their dispersed cloud of shared electrons. However, an obvious physical mismatch occurs when inserting metal electrodes inside a living organism. Since these materials are not as soft as living tissues, internal damage followed by an immune response impacts the impedance of such probes.In the late 80s', the large-scale commercialization of water processable conducting polymers brought a new paradigm in the choice of electronic material for bioelectronics devices. Compared to metals, conducting polymers are composed of semi-crystalline blocks that interact through electrostatic forces. These soft structures make these materials permeable to aqueous solutions, which allow the introduction of ionic species in the vicinity of the polymer backbone. Ions close to the polymer backbone can tune the conductivity of the material creating a unique ion/electron dialogue that increases the electronic signal resolution. Additionally, these soft structures considerably reduce scaring effects and therefore enable the devices to trigger lower immune responses. Conducting polymers could also be directly inserted within living tissues to create electronic platforms inside a host. Living organisms with new material properties could unravel new functions such as collecting electrophysiological data without surgery.Plants are living organisms that made their way out of the ocean and conquered most of the available land on earth. Saying that plants are good climate controllers is a euphemism since plants are legitimately the organisms that have settled the climate conditions for the development of more advanced life forms. Plant biohybrid is a new technological concept where plants are not only seen for their nutritious or environmental aspect but also as devices that can record and transfer information about their local environmental conditions. Such data could be used in a positive feedback loop to improve the production yield of crops or understand the underlying communication mechanism that occurs between plants or with plant micro-biomes. Most of the approaches toward plant biohybrids nowadays focus on nanomaterials that act as fluorescent probes in leaves and detect analytes from plants' local environment.In this thesis, we push forward a plant biohybrid strategy that instead uses conducting polymers as vectors to build conductors inside plants with the aim to build electrochemical platforms that could be used for applications such as energy storage, sensing, and energy production. Works developed in this thesis are going in an array of directions that aims for the better integration of electronic platforms in living systems with more focus on plants.We first identified a plant enzymatic mechanism that triggers the polymerization of a thiophene oligomer, namely ETE-S in vivo and in vitro. Such plant enzymatic pathways can then be reused to develop electronic systems in plantae without additional reagents. In the next work, we presented the synthesis of three new oligomers called ETE-N, EEE-S, and EEE-N that have a similar architecture compared to ETE-S but with different chemical moieties such as a different ionic side chain or an EDOT instead of thiophene in the middle position of the oligomer. We then demonstrated the effective enzymatic polymerization of these oligomers both in vivo and in vitro and how the resulting polymers' optoelectronic and tissue integrations properties differ. Towards even more versatility, we demonstrated that this electronic integration in vivo was also observed in the case of an animal: the freshwater hydra polyp. The polymerization was observed mostly in differentiated cells from the gastric column of the animal that normally secretes an adhesive used to fix the animal underwater. P(ETE-S) was incorporated in this glue that we managed to characterize using electrochemical methods. Lastly, we performed demonstrations of electrochemical applications with a plant root system. By dipping several roots in an ETE-S solution, we created a network of conducting roots that can effectively store charge as a capacitor with performance comparable to what is classically obtained with conducting polymers. In addition, we modified roots with two different surface modification concepts to make them specific to glucose oxidation: the first method uses a traditional redox hydrogel with a crosslinker and glucose oxidase. The second one uses the embedment of a glucosespecific enzyme inside the p(ETE-S) layer during its formation. These devices are presented as possible new solutions for environmental glucose sensors that could collect current from the environment and store it in neighbouring capacitive roots.Overall, this thesis shows that the enzymatic activity of living systems can be used from an engineering point of view as part of a deposition methods for the development of biohybrid applications.
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| 4. |
- Mantione, Daniele, et al.
(författare)
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Thiophene-Based Trimers for In Vivo Electronic Functionalization of Tissues
- 2020
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Ingår i: ACS APPLIED ELECTRONIC MATERIALS. - : AMER CHEMICAL SOC. - 2637-6113. ; 2:12, s. 4065-4071
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Tidskriftsartikel (refereegranskat)abstract
- Electronic materials that can self-organize in vivo and form functional components along the tissue of interest can result in a seamless integration of the bioelectronic interface. Previously, we presented in vivo polymerization of the conjugated oligomer ETE-S in plants, forming conductors along the plant structure. The EDOT-thiophene-EDOT trimer with a sulfonate side group polymerized due to the native enzymatic activity of the plant and integrated within the plant cell wall. Here, we present the synthesis of three different conjugated trimers based on thiophene and EDOT or purely EDOT trimers that are able to polymerize enzymatically in physiological pH in vitro as well as in vivo along the roots of living plants. We show that by modulating the backbone and the side chain, we can tune the electronic properties of the resulting polymers as well as their localization and penetration within the root. Our work paves the way for the rational design of electronic materials that can self-organize in vivo for spatially controlled electronic functionalization of living tissue.
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| 5. |
- Parker, Daniela, et al.
(författare)
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Biohybrid plants with electronic roots via in vivo polymerization of conjugated oligomers
- 2021
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Ingår i: Materials Horizons. - : Royal Society of Chemistry. - 2051-6347 .- 2051-6355. ; 8:12, s. 3295-3305
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Tidskriftsartikel (refereegranskat)abstract
- Plant processes, ranging from photosynthesis through production of biomaterials to environmental sensing and adaptation, can be used in technology via integration of functional materials and devices. Previously, plants with integrated organic electronic devices and circuits distributed in their vascular tissue and organs have been demonstrated. To circumvent biological barriers, and thereby access the internal tissue, plant cuttings were used, which resulted in biohybrids with limited lifetime and use. Here, we report intact plants with electronic functionality that continue to grow and develop enabling plant-biohybrid systems that fully maintain their biological processes. The biocatalytic machinery of the plant cell wall was leveraged to seamlessly integrate conductors with mixed ionic-electronic conductivity along the root system of the plants. Cell wall peroxidases catalyzed ETE-S polymerization while the plant tissue served as the template, organizing the polymer in a favorable manner. The conductivity of the resulting p(ETE-S) roots reached the order of 10 S cm(-1) and remained stable over the course of 4 weeks while the roots continued to grow. The p(ETE-S) roots were used to build supercapacitors that outperform previous plant-biohybrid charge storage demonstrations. Plants were not affected by the electronic functionalization but adapted to this new hybrid state by developing a more complex root system. Biohybrid plants with electronic roots pave the way for autonomous systems with potential applications in energy, sensing and robotics.
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| 6. |
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| 7. |
- Stavrinidou, Eleni, et al.
(författare)
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Plant Bioelectronics and Biohybrids : The Growing Contribution of Organic Electronic and Carbon-Based Materials
- 2022
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Ingår i: Chemical Reviews. - : American Chemical Society (ACS). - 0009-2665 .- 1520-6890. ; 122:4, s. 4847-4883
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Forskningsöversikt (refereegranskat)abstract
- Life in our planet is highly dependent on plants as they are the primary source of food, regulators of the atmosphere, and providers of a variety of materials. In this work, we review the progress on bioelectronic devices for plants and biohybrid systems based on plants, therefore discussing advancements that view plants either from a biological or a technological perspective, respectively. We give an overview on wearable and implantable bioelectronic devices for monitoring and modulating plant physiology that can be used as tools in basic plant science or find application in agriculture. Furthermore, we discuss plant wearable devices for monitoring a plants microenvironment that will enable optimization of growth conditions. The review then covers plant biohybrid systems where plants are an integral part of devices or are converted to devices upon functionalization with smart materials, including self-organized electronics, plant nanobionics, and energy applications. The review focuses on advancements based on organic electronic and carbon-based materials and discusses opportunities, challenges, as well as future steps.
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| 8. |
- Tommasini, Giuseppina, et al.
(författare)
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In vivo neuromodulation of animal behavior with organic semiconducting oligomers
- 2023
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Ingår i: Science Advances. - : AMER ASSOC ADVANCEMENT SCIENCE. - 2375-2548. ; 9:42
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Tidskriftsartikel (refereegranskat)abstract
- Modulating neural activity with electrical or chemical stimulus can be used for fundamental and applied research. Typically, neuronal stimulation is performed with intracellular and extracellular electrodes that deliver brief electrical pulses to neurons. However, alternative wireless methodologies based on functional materials may allow clinical translation of technologies to modulate neuronal function. Here, we show that the organic semiconducting oligomer 4-[2-{2,5-bis(2,3-dihydrothieno[3,4-b][1,4]dioxin-5-yl)thiophen-3-yl}ethoxy]butane-1-sulfonate (ETE-S) induces precise behaviors in the small invertebrate Hydra, which were dissected through pharmacological and electrophysiological approaches. ETE-S-induced behavioral response relies on the presence of head neurons and calcium ions and is prevented by drugs targeting ionotropic channels and muscle contraction. Moreover, ETE-S affects Hydras electrical activity enhancing the contraction burst frequency. The unexpected neuromodulatory function played by this conjugated oligomer on a simple nerve net opens intriguing research possibilities on fundamental chemical and physical phenomena behind organic bioelectronic interfaces for neuromodulation and on alternative methods that could catalyze a wide expansion of this rising technology for clinical applications.
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| 9. |
- Tommasini, Giuseppina, et al.
(författare)
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Seamless integration of bioelectronic interface in an animal model via in vivo polymerization of conjugated oligomers
- 2022
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Ingår i: Bioactive Materials. - : Elsevier BV. - 2452-199X. ; 10, s. 107-116
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Tidskriftsartikel (refereegranskat)abstract
- Leveraging the biocatalytic machinery of living organisms for fabricating functional bioelectronic interfaces, in vivo, defines a new class of micro-biohybrids enabling the seamless integration of technology with living biological systems. Previously, we have demonstrated the in vivo polymerization of conjugated oligomers forming conductors within the structures of plants. Here, we expand this concept by reporting that Hydra, an invertebrate animal, polymerizes the conjugated oligomer ETE-S both within cells that expresses peroxidase activity and within the adhesive material that is secreted to promote underwater surface adhesion. The resulting conjugated polymer forms electronically conducting and electrochemically active μm-sized domains, which are inter-connected resulting in percolative conduction pathways extending beyond 100 μm, that are fully integrated within the Hydra tissue and the secreted mucus. Furthermore, the introduction and in vivo polymerization of ETE-S can be used as a biochemical marker to follow the dynamics of Hydra budding (reproduction) and regeneration. This work paves the way for well-defined self-organized electronics in animal tissue to modulate biological functions and in vivo biofabrication of hybrid functional materials and devices.
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