The Effect of Organic Semiconductor Electron Affinity on Preventing Parasitic Oxidation Reactions Limiting Performance of n‐Type Organic Electrochemical Transistors

A key challenge in the development of organic mixed ionic-electronic conducting materials (OMIEC) for high performance electrochemical transistors is their stable performance in ambient. When operating in aqueous electrolyte, potential reactions of the electrochemically injected electrons with air and water could hinder their persistence, leading to a reduction in charge transport. Here, the impact of deepening the LUMO energy level of a series of electron-transporting semiconducting polymers is evaluated, and subsequently rendering the most common oxidation processes of electron polarons thermodynamically unfavorable, on organic electrochemical transistors (OECTs) performance. Employing time resolved spectroelectrochemistry with three analogous polymers having varying electron affinities (EA), it is found that an EA below the thermodynamic threshold for oxidation of its electron polarons by oxygen significantly improves electron transport and lifetime in air. A polymer with a sufficiently large EA and subsequent thermodynamically unfavorable oxidation of electron polarons is reported, which is used as the semiconducting layer in an OECT, in its neutral and N-DMBI doped form, resulting in an excellent and air-stable OECT performance. These results show a general design methodology to avoid detrimental parasitic reactions under ambient conditions, and the benefits that arise in electrical performance.

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Publication Details

Journal
Advanced Materials
Published
2024-09-02
DOI
https://doi.org/10.1002/adma.202403911
Citations
17
Primary Topic
Conducting polymers and applications
Type
article
Field-Weighted Citation Impact
2.87

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article

The Effect of Organic Semiconductor Electron Affinity on Preventing Parasitic Oxidation Reactions Limiting Performance of n‐Type Organic Electrochemical Transistors

Maryam Alsufyani, Benjamin Moss, Ruiheng Wu, Alexandra F. Paterson et al.
17 citations
Advanced Materials
Conducting polymers and applications
2.87
article

The Effect of Organic Semiconductor Electron Affinity on Preventing Parasitic Oxidation Reactions Limiting Performance of n‐Type Organic Electrochemical Transistors

Maryam Alsufyani, Benjamin Moss, Ruiheng Wu, Alexandra F. Paterson, Maryam Shahi, Claudia E. Tait, Karl J. Thorley, William K. Myers, Reem B. Rashid, Dilara Meli, Iain McCulloch, Craig Combe, Sahika Inal, Jonathan Rivnay, Grant A. D. Ritchie, Sang Young Jeong, Han Young Woo, Bryan D. Paulsen, James Robert Durrant, Yuanbao Lin, Ji‐Seon Kim, Xiaolei Zhao, Katherine Stewart, Charlie Kniebe‐Evans
article en
17 citations

Abstract

A key challenge in the development of organic mixed ionic-electronic conducting materials (OMIEC) for high performance electrochemical transistors is their stable performance in ambient. When operating in aqueous electrolyte, potential reactions of the electrochemically injected electrons with air and water could hinder their persistence, leading to a reduction in charge transport. Here, the impact of deepening the LUMO energy level of a series of electron-transporting semiconducting polymers is evaluated, and subsequently rendering the most common oxidation processes of electron polarons thermodynamically unfavorable, on organic electrochemical transistors (OECTs) performance. Employing time resolved spectroelectrochemistry with three analogous polymers having varying electron affinities (EA), it is found that an EA below the thermodynamic threshold for oxidation of its electron polarons by oxygen significantly improves electron transport and lifetime in air. A polymer with a sufficiently large EA and subsequent thermodynamically unfavorable oxidation of electron polarons is reported, which is used as the semiconducting layer in an OECT, in its neutral and N-DMBI doped form, resulting in an excellent and air-stable OECT performance. These results show a general design methodology to avoid detrimental parasitic reactions under ambient conditions, and the benefits that arise in electrical performance.

Advanced MaterialsVol. 36(44)
Northwestern University (US), University of Kentucky (US), Shanghai Jiao Tong University (CN), Korea University (KR), Hong Kong University of Science and Technology (HK), Princeton University (US), University of Oxford (GB), Education University of Hong Kong (HK), Imperial College London (GB), King Abdullah University of Science and Technology (SA), University of Hong Kong (HK)
National Science Foundation, W. M. Keck Foundation, Northwestern University, Royal Society, Imperial College London, National Research Foundation, National Research Foundation of Korea, King Abdullah University of Science and Technology, International Institute for Nanotechnology, Northwestern University, Engineering and Physical Sciences Research Council, Division of Materials Research, Division of Electrical, Communications and Cyber Systems
Clean water and sanitation
Openalex Percentile: Top 8%
Conducting polymers and applications
2.87
DOIOpen Access PDFOpenAlex
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