Sequential Cyanation of Polythiophenes: Tuning Charge Carrier Polarity in Organic Electrochemical Transistors

Ma，Suxiang1; Wang，Junwei1; Wu，Wenchang1; Wu，Ziang2; Zhang，Hao3; Chen，Rifei1; Liu，Bin1; Feng，Kui1,4; Woo，Han Young2; Guo，Xugang1,5

2023

10.1002/aelm.202300207

Advanced Electronic Materials   Impact Factor & Quartile

2199-160X

2199-160X

Polythiophenes, built on head-to-head (HH) linked 3,3′-oligomer ethylene glycol-2,2′-bithiophene (gT2), have simple chemical structure, good backbone planarity, and relatively high-lying the lowest unoccupied molecular orbital (LUMO) energy levels, hence showing excellent p-type performance in organic electrochemical transistors (OECTs) with µC* of several hundred F cm V s. In this study, sequential cyano substitution is utilized to enable transformation of charge carrier polarity from p-type to n-type in OECTs, based on the parent polythiophene g4T2-T2. With the increase of cyano group number, the polythiophenes exhibit gradually lowered LUMO levels from −2.55 to −3.90 eV. As a result, from g4T2-T2 to CNg4T2-CNT2, the p-type performance dramatically diminishes accomplished by the enhancement of n-type one when applied in OECTs. To the authors' delight, polymer CNg4T2-CNT2 with the highest content of cyano groups exhibits a remarkable n-type µC* of 27.01 F cm V s and high g of 6.75 S cm with negligible p-type character. This study demonstrates that sequential cyano substitution provides a powerful approach for developing high-performance n-type polymers for OECT applications.

charge carrier polarity cyanation organic electrochemical transistors organic mixed ionic–electronic conductors polythiophene

SCI

English

First ; Corresponding

Songshan Lake Materials Laboratory[2021SLABFK03] ; Shenzhen Innovation Commission of Science and Technology[JCYJ20220818100617037] ; National Natural Science Foundation of China["22275078","22005135"] ; National Research Foundation of Korea["2019R1A6A1A11044070","2020M3H4A3081814"]

Science & Technology - Other Topics ; Materials Science ; Physics

Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied

WOS:001060851900001

WILEY

2-s2.0-85170060653

Scopus

1.Department of Materials Science and Engineering,Southern University of Science and Technology (SUSTech),Shenzhen,Guangdong,518055,China
2.Department of Chemistry,Korea University,Seoul,136-713,South Korea
3.Department of Chemistry,Southern University of Science and Technology (SUSTech),Shenzhen,Guangdong,518055,China
4.Academy for Advanced Interdisciplinary Studies,Southern University of Science and Technology (SUSTech),Shenzhen,Guangdong,518055,China
5.Songshan Lake Materials Laboratory,Dongguan,Guangdong,523808,China

Ma，Suxiang,Wang，Junwei,Wu，Wenchang,et al. Sequential Cyanation of Polythiophenes: Tuning Charge Carrier Polarity in Organic Electrochemical Transistors[J]. Advanced Electronic Materials,2023.

Ma，Suxiang.,Wang，Junwei.,Wu，Wenchang.,Wu，Ziang.,Zhang，Hao.,...&Guo，Xugang.(2023).Sequential Cyanation of Polythiophenes: Tuning Charge Carrier Polarity in Organic Electrochemical Transistors.Advanced Electronic Materials.

Ma，Suxiang,et al."Sequential Cyanation of Polythiophenes: Tuning Charge Carrier Polarity in Organic Electrochemical Transistors".Advanced Electronic Materials (2023).