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Peer-reviewedCC BYJournal of the American Chemical Society

Myelin Sheath-Inspired Fluorocarbon Hydrophobic Bridges for Stable n-Type Organic Mixed Ionic-Electronic Conductors.

4 affiliations
  1. 1Key Laboratory of Medicinal Chemistry for Natural Resource, Ministry of Education, School of Chemical Science and Technology, Yunnan University, Kunming650091, China.
  2. 2School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, Georgia30332, United States.
  3. 3Southwest United Graduate School, Kunming650092, China.
  4. 4Department of Materials, The Hong Kong University of Science and Technology, Hong Kong999077, China.

Abstract

Operationally stable n-type organic mixed ionic-electronic conductors (OMIECs) remain a critical bottleneck for organic electrochemical transistors (OECTs) for application in bioelectronic and neuromorphic devices. However, several state-of-the-art n-type OMIECs suffer from performance decay and poor stability when operated in aqueous media. Inspired by myelin sheaths, we challenge the conventional "π-backbone + hydrophilic side-chain" design and propose a molecular architecture with fluorocarbon hydrophobic bridges to spatially segregate, at the molecular level, ionic and electronic pathways. By tuning the fluorocarbon bridge chain length in fluorocarbon-ethylene glycol chain substituents [-CH2(CF2)nCH2(OCH2CH2)5OMe = 2nFG; n = 1, 2, 3, 4, 6] of a DPP-CNTVT polymer series (2nFG-P), we balance electron transport, ion exchange, redox chemistry efficiency, and water incorporation. Extensive in situ spectroelectrochemistry, EIS, Raman, EQCM-D, AFM, and GIWAXS characterization reveals that tuning the length of the hydrophobic bridge enables good electron transport, suppresses excessive water incorporation, and enhances stability. Thus, the polymer with a mid-length bridge, 8FG-P (n = 4), achieves the greatest electron transport (μC* ∼ 157 F cm-1 V-1 s-1, μ ∼ 1.22 cm2 V-1 s-1), fastest response (τon/τoff = 2.6/1.5 ms), and retains >90% of the initial performance after 10,000 s of operation in water, a result independent of the polymer molecular weight. This strategy potentially expands OMIECs design principles and offers useful insights toward stable n-type OECT semiconductors.

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BibTeX
@article{feng2026myelin,
  title = {{Myelin Sheath-Inspired Fluorocarbon Hydrophobic Bridges for Stable n-Type Organic Mixed Ionic-Electronic Conductors.}},
  author = {Wang Feng and Shaodan Cai and Chao Deng and Bei Zhang and Mengge Wu and Jianhua Chen and Antonio Facchetti},
  journal = {Journal of the American Chemical Society},
  year = {2026},
  month = oct,
  doi = {10.1021/jacs.6c12196},
  url = {https://europepmc.org/article/MED/42912344},
  note = {CC BY},
}
RIS
TY  - JOUR
TI  - Myelin Sheath-Inspired Fluorocarbon Hydrophobic Bridges for Stable n-Type Organic Mixed Ionic-Electronic Conductors.
AU  - Wang Feng
AU  - Shaodan Cai
AU  - Chao Deng
AU  - Bei Zhang
AU  - Mengge Wu
AU  - Jianhua Chen
AU  - Antonio Facchetti
PY  - 2026
DA  - 2026/10/01
JO  - Journal of the American Chemical Society
DO  - 10.1021/jacs.6c12196
UR  - https://europepmc.org/article/MED/42912344
AB  - Operationally stable n-type organic mixed ionic-electronic conductors (OMIECs) remain a critical bottleneck for organic electrochemical transistors (OECTs) for application in bioelectronic and neuromorphic devices. However, several state-of-the-art n-type OMIECs suffer from performance decay and poor stability when operated in aqueous media. Inspired by myelin sheaths, we challenge the conventional "π-backbone + hydrophilic side-chain" design and propose a molecular architecture with fluorocarbon hydrophobic bridges to spatially segregate, at the molecular level, ionic and electronic pathways. By tuning the fluorocarbon bridge chain length in fluorocarbon-ethylene glycol chain substituents [-CH2(CF2)nCH2(OCH2CH2)5OMe = 2nFG; n = 1, 2, 3, 4, 6] of a DPP-CNTVT polymer series (2nFG-P), we balance electron transport, ion exchange, redox chemistry efficiency, and water incorporation. Extensive in situ spectroelectrochemistry, EIS, Raman, EQCM-D, AFM, and GIWAXS characterization reveals that tuning the length of the hydrophobic bridge enables good electron transport, suppresses excessive water incorporation, and enhances stability. Thus, the polymer with a mid-length bridge, 8FG-P (n = 4), achieves the greatest electron transport (μC* ∼ 157 F cm-1 V-1 s-1, μ ∼ 1.22 cm2 V-1 s-1), fastest response (τon/τoff = 2.6/1.5 ms), and retains >90% of the initial performance after 10,000 s of operation in water, a result independent of the polymer molecular weight. This strategy potentially expands OMIECs design principles and offers useful insights toward stable n-type OECT semiconductors.
SN  - 0002-7863
SN  - 1520-5126
ER  -