Controlling ions and electrons in aqueous solution: an alternative point of view of the charge-transport behavior of eumelanin-inspired material

Paulin, João Vitor; Pereira, Mariane P.; Bregadiolli, Bruna Andressa; Cachaneski-Lopes, João; Graeff, Carlos F. O.; Batagin‐Neto, Augusto; Bufon, Carlos César Bof

doi:10.1039/d3tc00490b

J. Mater. Chem. C

2023

DOI: 10.1039/d3tc00490b

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Controlling ions and electrons in aqueous solution: an alternative point of view of the charge-transport behavior of eumelanin-inspired material

João Vitor Paulin

Mariane P. Pereira

Bruna Andressa Bregadiolli

et al.

Abstract: The possibility of current injection and transport in eumelanin films, humans' most common natural pigment, has fascinated physicists and materials scientists since the early '60s. Nowadays, it is accepted that...

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Cited by 8 publications

(28 citation statements)

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“…This response indicates that water affects the electrochemical behavior at the electrodes, improving the charge transfer and decreasing the electrode polarization. This behavior is compatible with eumelanin-inspired materials’ recently speculated electrochemical doping mechanism …”

supporting

confidence: 83%

“…This behavior is compatible with eumelanininspired materials' recently speculated electrochemical doping mechanism. 9 Taking into consideration the ionic-electronic nature of this system, we estimate the specific capacitance (C) using 22…”

mentioning

confidence: 99%

“…While a substantial number of studies have predominantly focused on synthetic analogs, these explorations have shed light on the underlying principles of charge transport mechanisms. Nonetheless, there remains a significant lack of comprehensive investigation into the charge transport behavior of eumelanin within its natural context. − …”

mentioning

confidence: 99%

“…This behavior implies that a Randles circuit, schematically reported in Figure S5, can be an appropriate model for the N-EuM analysis. The Randles model, which has been used for eumelanin characterization, ,,,, considers a contact resistance between the IDE and N-EuM, a dielectric double layer, an ionic dissipation current, and the diffusion of protons at the blocking electrode surface. Table S1 reports the obtained fitting parameters.…”

mentioning

confidence: 99%

“…To further analyze the protonic behavior of N-EuM, the dielectric permittivity response (ε) as a function of frequency was calculated from the real ( Z′ ) and imaginary ( Z″ ) parts of the impedance following ε = ε R + j ε I , , with ε R = 1 ω C 0 − Z ″ false| Z false| 2 ε I = 1 ω C 0 Z ′ false| Z false| 2 …”

mentioning

confidence: 99%

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Exploring the Charge Transport of a Natural Eumelanin for Sustainable Technologies

Paulin,

Bayram,

Graeff

et al. 2023

ACS Appl. Bio Mater.

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Eumelanin, the main quinone-based biomaterial of the melanin family of compounds, is emerging as a model for medical and sustainable electronic interfaces due to its biocompatibility, biodegradability, and transducing abilities. The study utilizes current–voltage measurements and impedance/dielectric spectroscopy under a controlled hydration atmosphere to investigate the charge transport of eumelanin produced from the S. parvus BSB49 strain. We show no differences in the electrical response in highly hydrated conditions compared to the standard synthetic eumelanin. Hence, our findings provide the groundwork to assess the potential use of this natural eumelanin in sustainable organic (bio)electronic applications.

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supporting

confidence: 83%

mentioning

confidence: 99%

mentioning

confidence: 99%

mentioning

confidence: 99%

mentioning

confidence: 99%

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Exploring the Charge Transport of a Natural Eumelanin for Sustainable Technologies

Paulin,

Bayram,

Graeff

et al. 2023

ACS Appl. Bio Mater.

Self Cite

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Electrochemical behavior of non‐functionalized and sulfonated melanins at different pH values

Brizuela Guerra,

Lima,

Paulin

et al. 2024

Polymer International

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Melanins are macromolecular pigments widely spread in many living organisms, with unique physical and chemical properties. Specifically, their conductive properties have drawn attention for applications in different devices; however, the electrochemical response is equally necessary for designing technologies in sustainable bioelectronics. In this sense, we report a comparative study of the redox electrochemical properties of non‐functionalized and sulfonated melanins in different pH environments. The electrochemical response was investigated using cyclic voltammetry, electrochemical impedance spectroscopy, dielectric permittivity and AC/DC conductivity at pH 3, 5 and 7. The voltammetric currents were higher at low pH, in agreement with the known proton transport properties of melanins. The effect of pH on electrochemical properties was slightly more significant in non‐functionalized pigments. Melanins with a higher 5,6‐dihydroxyindole carboxylic acid/5,6‐dihydroxyindole ratio showed high DC current and low impedance. No significant difference was observed in the dielectric relaxation process between the different samples. © 2024 Society of Chemical Industry.

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Electrochemical Doping Effect on the Conductivity of Melanin-Inspired Materials

Brizuela Guerra,

Morais Lima,

Nozella

et al. 2024

ACS Appl. Bio Mater.

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Eumelanin is a natural pigment that can be particularly valuable for sustainable bioelectronic devices due to its inherent biocompatibility and hydration-dependent conductivity. However, the low conductivity of eumelanin limits its technological development. In this research, electrochemical doping was proposed as an alternative route to increase the electronic conductivity of synthetic eumelanin derivatives. Thin films of sulfonated eumelanin were deposited on platinum interdigitated electrodes and electrochemically treated by using cyclic voltammetry and chronoamperometry treatments. X-ray photoelectron spectroscopy analysis confirmed ion doping in sulfonated melanin. Current−voltage, current−time, and electrochemical impedance measurements were used to investigate the effect of different aqueous electrolytes (including KCl and LiClO 4 ) treatments on the charge transport of sulfonated eumelanin. We show that the conductivity depends on the type and size of the anion used and can reach 10 −3 S•cm −1 . Additionally, depending on the electrolyte, there is a change in charge transport from mixed ionic/electronic to a predominantly electronic-only conduction. Our results show that the chemical nature of the ion plays an important role in the electrochemical doping and, consequently, in the charge transport of eumelanin. These insights serve as inspiration to explore the use of alternative electrolytes with different compositions further and develop eumelanin-based devices with tunable conductivities.

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Controlling ions and electrons in aqueous solution: an alternative point of view of the charge-transport behavior of eumelanin-inspired material

Abstract: The possibility of current injection and transport in eumelanin films, humans' most common natural pigment, has fascinated physicists and materials scientists since the early '60s. Nowadays, it is accepted that...

Cited by 8 publications

References 102 publications

Exploring the Charge Transport of a Natural Eumelanin for Sustainable Technologies

Exploring the Charge Transport of a Natural Eumelanin for Sustainable Technologies

Electrochemical behavior of non‐functionalized and sulfonated melanins at different pH values

Electrochemical Doping Effect on the Conductivity of Melanin-Inspired Materials

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