Wireless Control of Redox Gradients in Conductive Hydrogels: A New Frontier in Drug Delivery & Energy Harvesting

Bipolar electrochemistry (BE) enables wireless redox control on conductive materials. Here, we use BE to create reversible redox gradients in PEDOT–alginate hydrogels, enabling targeted drug loading and energy harvesting. This approach bridges bioelectronics, and sustainable energy applications.
Wireless Control of Redox Gradients in Conductive Hydrogels: A New Frontier in Drug Delivery & Energy Harvesting
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Bipolar electrochemistry enables the wireless modulation of redox states across conductive materials, offering new possibilities for localized electrochemical transformations without the need for direct electrical connections. By leveraging this principle, we developed a system where redox gradients can be precisely controlled, opening pathways for novel applications in bioelectronics and materials science. Our study demonstrates how BE can be harnessed to manipulate the chemical and physical properties of conductive polymer-hydrogel hybrids, paving the way for innovative functional materials with tunable characteristics.

We are excited to share our latest publication exploring bipolar electrochemistry (BE) as a wireless strategy to spatially control redox gradients in conductive polymer-hydrogel hybrids (Figure 1)!

 a Chemical  reactions involving the electropolymerization of EDOT (blue dashed square),  resulting in a mixture of neutral PEDOT (benzoid structure) and oxidized PEDOT  (quinoid structure, depicted in blue). The redox equilibrium can be controlled via  bipolar (wireless) electrochemistry (red dashed square). b Schematic representation  of the bipolar electrochemical cell, where the PEDOT film electrodeposited on a  f  lexible ITO/PET substrate serves as the BPE. c Top-view schematic representation  of the bipolar electrochemical cell: water hydrolysis reactions at the driving elec trodes are depicted on each side, while the redox reaction of PEDOT occurs at the  BPE. d Image of the PEDOT film after the bipolar activation: oxidized PEDOT on  the left and reduced PEDOT on the right.
Fig. 1 | Conducting Polymer Films and Bipolar Electrochemistry. a Chemical  reactions involving the electropolymerization of EDOT (blue dashed square),  resulting in a mixture of neutral PEDOT (benzoid structure) and oxidized PEDOT  (quinoid structure, depicted in blue). The redox equilibrium can be controlled via  bipolar (wireless) electrochemistry (red dashed square). b Schematic representation  of the bipolar electrochemical cell, where the PEDOT film electrodeposited on a  flexible ITO/PET substrate serves as the BPE. c Top-view schematic representation  of the bipolar electrochemical cell: water hydrolysis reactions at the driving electrodes are depicted on each side, while the redox reaction of PEDOT occurs at the  BPE. d Image of the PEDOT film after the bipolar activation: oxidized PEDOT on the left and reduced PEDOT on the right.

By integrating poly(3,4-ethylenedioxythiophene) (PEDOT) with alginate hydrogels, we developed flexible bipolar electrodes (BPEs) capable of wireless and reversible redox tuning (Figure 2). This unique combination of a conductive polymer and biocompatible hydrogel matrix provides a mechanically adaptable platform for dynamic redox control. (10.20517/ss.2022.25; 10.1002/mame.202300263) The wireless nature of the system allows for seamless integration into biomedical and electronic devices, facilitating localized electrochemical processes in a completely untethered manner. This approach holds great promise for applications requiring spatially controlled chemical reactions, from responsive biointerfaces to advanced energy storage solutions.

 Fig. 2 | Hybrid Hydrogel Coating as BPEs.  a Chemical reactions involved in single-step electrodeposition of the conductive hybrid hydrogel: (1) Electropolymerization of EDOT (blue dashed square) to the mixture between neutral state of
 PEDOT (benzoid structure) and oxidized PEDOT (quinoid structure, represented in blue). PEDOT electropolymerization takes place in parallel with (2) decomposition of calcium carbonate, and (3) complexation with alginate macromolecules,
 resulting in formation of the alginate hydrogel (green dashed square). The redox equilibrium of PEDOT can be subsequently controlled by bipolar (wireless) electrochemistry. b Pictures of: (i) the entire BPE subjected to bending, and (ii) the oxidized (left) and reduced (right) sides following BE activation. c The 10th cycle of CV for the bare ITO/ PET (black), PEDOT/Alginateox (light blue) and PEDOT/Alginatered (dark blue), recorded in PBS at 50 mVs−1. d Nyquist plot of EIS for the PEDOT/Alginateox (light blue) and PEDOT/Alginatered (dark blue), recorded in PBS. e PEDOT resistance obtained from EIS for oxidized (right) and reduced (left) halves. f Charge storage capacity of reduced and oxidized BPE halves was obtained by applying +1.2 V or −0.8V (vs Ag/AgCl/KCl 3M) respectively for 30 min while measuring the resulting currents. Later, the BPEs were electronically reconnected using a new copper tape and placed back in the bipolar electrochemical cell as BPE electrode for a new cycle (n. 1, 2 and 3). g Wet mass(left) and dry (right) mass of hydrogels in the oxidized (light blue)
 and reduced (dark blue) halves of the BPE. h Water content in the oxidized (light blue) and reduced (dark blue) halves of the BPE. Error bars in (e–h) are standard deviations (see “Methods”).

🔹 Targeted drug loading – Fluorescein molecules were selectively loaded into specific regions of the hydrogel, demonstrating an alternative to conventional uniform doping techniques (Figure 3). This technique enables spatial control over the incorporation of bioactive molecules, allowing for the development of next-generation drug delivery systems. By leveraging BE, we demonstrate how wireless modulation can be used to create patterned drug reservoirs, which can be released in a controlled manner. This advancement is particularly relevant for precision medicine, where localized and programmable drug release is critical for improving therapeutic outcomes.

a Schematic representation of the  BPE (PET/ITO/PEDOT/Alginate hydrogel) wirelessly loaded with fluorescein  molecules (red dashed square), where (i) represents the initial state of the intact BPE  fully loaded with fluorescein molecules, (ii) represents passive (diffusion-con trolled), and (iii) electrically controlled release from Alginate and PEDOT layers of  the BPE halves. b Concentration of fluorescein passively released from the oxidized  (light blue) and reduced (dark blue) halves of the BPE. c Nyquist EIS plots of a BPE  (oxidized half) during passive fluorescein release. d Passive release profile (black,  n=4) and total impedance (red, n=1) vs time for the oxidized half of a BPE.  e Quantification of electrically driven release from oxidized (light blue) and reduced  (dark blue) halves of a BPE. f Profile of electrically driven release from the oxidized  half ofaBPE.Applicationofcontinuous−0.8 V(vsAg/AgCl/KCl3 M)orpulsed(8 s  at −0.8V) potential results in control of the release kinetics, n = 3. Error bars in  b, d–f are standard deviations (see “Methods”).
 Fig. 3 | Wireless Loading of Small Molecules. a Schematic representation of the BPE (PET/ITO/PEDOT/Alginate hydrogel) wirelessly loaded with fluorescein molecules (red dashed square), where (i) represents the initial state of the intact BPE fully loaded with fluorescein molecules, (ii) represents passive (diffusion-controlled), and (iii) electrically controlled release from Alginate and PEDOT layers of the BPE halves. b Concentration of fluorescein passively released from the oxidized (light blue) and reduced (dark blue) halves of the BPE. c Nyquist EIS plots of a BPE (oxidized half) during passive fluorescein release. d Passive release profile (black, n=4) and total impedance (red, n=1) vs time for the oxidized half of a BPE. e Quantification of electrically driven release from oxidized (light blue) and reduced (dark blue) halves of a BPE. f Profile of electrically driven release from the oxidized half of a BPE. Application of continuous−0.8 V(vs Ag/AgCl/KCl3 M)or pulsed(8 s at −0.8V) potential results in control of the release kinetics, n = 3. Error bars in b, d–f are standard deviations (see “Methods”).

🔹 Energy harvesting – By cutting gradient-encoded BPEs and closing an external circuit, we recovered stored electrochemical energy using a concentration cell mechanism (Figure 4). This innovative approach transforms our conductive hydrogel system into a wireless energy storage platform, capable of harnessing and releasing stored charge based on redox potential differences. The ability to wirelessly charge and discharge these materials suggests potential applications in self-powered biosensors, flexible electronics, and even implantable medical devices requiring localized power sources.

 a Schematic representation  of the single-cell battery design with chloride naturally diffusing from the wirelessly  charged PEDOT/Alginateox. b Electrochemical half-cell cathodic reaction of  PEDOT/Alginateox. c Electrical potential generated over time for different electro lyte solutions: PBS buffer (black), 100 mM hydrochloric acid (red), and 100 mM  sodiumhydroxide(green). dGalvanostaticcharge-discharge curves for the different  electrolytes at 0.1 A g−1. e Schematic representation of the single-cell design using  3D-printed parts. f Schematic representation of an assembled single-cell.  g Photograph of three single-cell batteries connected in series to a multimeter  measuring the generated DC voltage.
 Fig. 4 | Wirelessly charged concentration cell battery. a Schematic representation of the single-cell battery design with chloride naturally diffusing from the wirelessly charged PEDOT/Alginateox. b Electrochemical half-cell cathodic reaction of
 PEDOT/Alginateox. c Electrical potential generated over time for different electrolyte solutions: PBS buffer (black), 100 mM hydrochloric acid (red), and 100 mM sodium hydroxide (green). d Galvanostatic charge-discharge curves for the different electrolytes at 0.1 A g−1. e Schematic representation of the single-cell design using 3D-printed parts. f Schematic representation of an assembled single-cell. g Photograph of three single-cell batteries connected in series to a multimeter measuring the generated DC voltage.

Using cyclic voltammetry, impedance spectroscopy, Raman microscopy, and XPS, we mapped distinct redox regions within the BPEs, providing insights into wireless bioelectronics applications. (10.1038/s41467-022-29037-6)

This work highlights the untapped potential of BE in biomedical and energy fields, bridging materials science, electrochemistry, and bioengineering for next-generation drug delivery and energy storage systems.

Looking forward to discussions with fellow researchers on how BE can revolutionize wireless chemical control in functional materials!

Read more: https://www.nature.com/articles/s43246-025-00750-1 / Bipolar electrochemistry-driven wireless drug loading and energy harvesting in conductive hybrid hydrogels | Communications Materials

#BipolarElectrochemistry #Bioelectronics #Hydrogels #DrugDelivery #EnergyHarvesting #MaterialsScience #Electrochemistry

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Gels and Hydrogels
Physical Sciences > Materials Science > Soft Materials > Gels and Hydrogels
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