On the fundamentals of organic mixed ionic/electronic conductors

Fabiano, Simone; Flagg, Lucas; Hidalgo Castillo, Tania C.; Inal, Sahika; Kaake, Loren G.; Kayser, Laure V.; Keene, Scott T.; Ludwigs, Sabine; Muller, Christian; Savoie, Brett M.; Lüssem, Björn; Lutkenhaus, Jodie L.; Matta, Micaela; Meli, Dilara; Patel, Shrayesh N.; Paulsen, Bryan D.; Rivnay, Jonathan; Surgailis, Jokubas

doi:10.1039/d3tc03058j

J. Mater. Chem. C

2023

DOI: 10.1039/d3tc03058j

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On the fundamentals of organic mixed ionic/electronic conductors

Simone Fabiano,

Lucas Flagg,

Tania C. Hidalgo Castillo

et al.

Abstract: The first Telluride Science meeting (formerly TSRC) on organic mixed ionic and electronic conductors (OMIECs), Oct 3-7, 2022, brought together researchers across the field to understand the fundamental processes and...

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2024

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Cited by 8 publications

References 118 publications

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Balancing Electroactive Backbone and Oligo(Ethylene Oxy) Side‐Chain Content Improves Stability and Performance of Soluble PEDOT Copolymers in Organic Electrochemical Transistors

Bardagot,

DiTullio,

Jones

et al. 2024

Adv Funct Materials

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The development of devices based on organic electrochemical transistors (OECTs) relies on the rational design of high‐performing organic mixed ionic‐electronic conductors (OMIECs). Here, a series of solution‐processable copolymers composed of unsubstituted 2,2′‐bis‐(3,4‐ethylenedioxy)thiophene (biEDOT) and 3,4‐propylenedioxythiophene (ProDOT) substituted with linear or branched oligo(ethylene oxy) (OE) side chains are reported. By varying the size of the linear and branched side chains, it is found that the highest OECT performance is achieved with a near equivalent molar mass of the side chain and electroactive conjugated polymer repeat unit. With four OE units (PE2‐OE4, electroactive content of 49%), OECTs with state‐of‐the‐art normalized transconductance (453 ± 70 S cm−1) and µC* (830 ± 37 F cm−1 V−1 s−1), rapid dedoping kinetics, and a pulsing stability of 99% IDS retention over 200 ON/OFF cycles are achieved. A consistent improvement in OECT stability with decreasing side‐chain size is also observed. The origin of the enhanced stability is rationalized by correlating IDS losses to changes in channel absorbance cycle after cycle during operation. This work encourages the calculation of the electroactive polymer content of an OMIEC when designing the side chains. It also shows that the PE2 backbone with short OE side chains is a promising structure for (bio)electrochemical devices.

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Balancing Electroactive Backbone and Oligo(Ethylene Oxy) Side‐Chain Content Improves Stability and Performance of Soluble PEDOT Copolymers in Organic Electrochemical Transistors

Bardagot,

DiTullio,

Jones

et al. 2024

Adv Funct Materials

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Flexible Composites from Water-Dispersible Components: Poly(vinyl alcohol), Janus Nanoparticles, and Polyaniline─Toward Mixed Ionic–Electronic Conductors

Asandulesa,

Solonaru,

Honciuc

et al. 2024

ACS Appl. Polym. Mater.

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As the demand for multifunctional materials increases within the realm of electronics and photonics, composites that support both ionic and electronic charge transports are emerging as a promising platform for the future generation of electronic materials and devices. This study develops and characterizes a green composite material, utilizing a nonconductive poly(vinyl alcohol) (PVA) matrix integrated with glycerol (Gly) for enhanced ionic conductivity and mechanical flexibility, amphiphilic Janus nanoparticles (JNPs), and in situ synthesized polyaniline (PANi). The incorporation of JNPs, modified to possess either insulating or semiconducting properties through a semiconducting PANi layer on one of the Janus lobes, and the synthesis of PANi within the composite matrix are key to achieving mixed ionic–electronic conductivity, crucial for advanced dielectric functionalities. Employing broadband dielectric spectroscopy, this study assesses the composite’s electrical and dielectric properties, focusing on the interplay and polarization mechanisms induced by each component. Results reveal that glycerol’s contribution to ionic conductivity through a hydrogen bond network is significant, while JNPs/PANi add distinct electronic transport pathways, indicating a complex yet effective charge transport system within the composite. The utilization of water as a solvent emphasizes the material’s suitability for environmentally sustainable applications in electronics and photonics, presenting its potential in next-generation device architectures.

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The hierarchical structure of organic mixed ionic–electronic conductors and its evolution in water

Tsarfati,

Bustillo,

Savitzky

et al. 2024

Nat. Mater.

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On the fundamentals of organic mixed ionic/electronic conductors

Abstract: The first Telluride Science meeting (formerly TSRC) on organic mixed ionic and electronic conductors (OMIECs), Oct 3-7, 2022, brought together researchers across the field to understand the fundamental processes and...

Cited by 8 publications

References 118 publications

Balancing Electroactive Backbone and Oligo(Ethylene Oxy) Side‐Chain Content Improves Stability and Performance of Soluble PEDOT Copolymers in Organic Electrochemical Transistors

Balancing Electroactive Backbone and Oligo(Ethylene Oxy) Side‐Chain Content Improves Stability and Performance of Soluble PEDOT Copolymers in Organic Electrochemical Transistors

Flexible Composites from Water-Dispersible Components: Poly(vinyl alcohol), Janus Nanoparticles, and Polyaniline─Toward Mixed Ionic–Electronic Conductors

The hierarchical structure of organic mixed ionic–electronic conductors and its evolution in water

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