Donor Engineering for High Performance n‐Type OECT Materials with Exceptional Operational Stability

R Riqing Ding (State Key Lab of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Functional and Intelligent Hybrid Materials and Devices, South China Advanced Institute for Soft Matter Science and Technology, School of Emergent Soft Matter South China University of Technology Guangzhou 510640 P.R. China) X Xiage Zhang Y Yidan Luan (State Key Lab of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Functional and Intelligent Hybrid Materials and Devices, South China Advanced Institute for Soft Matter Science and Technology, School of Emergent Soft Matter South China University of Technology Guangzhou 510640 P.R. China) M Meishan Peng (State Key Lab of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Functional and Intelligent Hybrid Materials and Devices, South China Advanced Institute for Soft Matter Science and Technology, School of Emergent Soft Matter South China University of Technology Guangzhou 510640 P.R. China) W Wantao Chen (State Key Lab of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Functional and Intelligent Hybrid Materials and Devices, South China Advanced Institute for Soft Matter Science and Technology, School of Emergent Soft Matter South China University of Technology Guangzhou 510640 P.R. China) S Sijing Wang S Shengyao Su S Shunyang Lu (State Key Lab of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Functional and Intelligent Hybrid Materials and Devices, South China Advanced Institute for Soft Matter Science and Technology, School of Emergent Soft Matter South China University of Technology Guangzhou 510640 P.R. China) S Sang Young Jeong (Department of Chemistry, Korea University, Anamro 145, Seoul 02841, Republic of Korea) H Han Young Woo X Xugang Guo (Department of Materials Science and Engineering) K Kui Feng (Department of Materials Science and Engineering) Z Zi‐Hao Guo (State Key Lab of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Functional and Intelligent Hybrid Materials and Devices, South China Advanced Institute for Soft Matter Science and Technology, School of Emergent Soft Matter South China University of Technology Guangzhou 510640 P.R. China)

Abstract

Abstract Donor–acceptor (D–A) conjugated polymeric mixed ionic–electronic conductors (PMIECs) have been widely used in organic electrochemical transistors (OECTs) due to their structural diversity and the tunability of their frontier molecular orbital (FMO) energy levels. However, the slower development of n‐type materials compared to p‐type ones limits their potential in advanced technological applications. In this study, we design and synthesize a novel thiophene‐based donor building block, 2,3‐di(thiophen‐2‐yl)fumaronitrile ( DTFMCN ), for D–A conjugated n‐type PMIECs through donor engineering strategies. DTFMCN can be easily synthesized from commercially available starting materials via a simple one‐step process. The DTFMCN‐based D–A conjugated polymers, S‐DTFMCN and B‐DTFMCN , exhibit extremely low‐lying lowest unoccupied molecular orbital (LUMO) energy levels and show typical n‐type characteristics. OECT devices based on these polymers demonstrate ultra‐low threshold voltages (6 and 40 mV) and high µ C* values of 13.49 and 13.57 F cm −1  V −1  s −1 , respectively. More importantly, these devices exhibit exceptionally high operational stability; the current retention rate after 168 minutes of operation is 96%, making them one of the most stable n‐type OECT devices reported to date. This study highlights the effectiveness of DTFMCN in improving the operational stability of n‐type OECT devices, offering promising potential for applications in bioelectronics.

Article Details

Volume / Issue Vol. 64, Issue 36
Published September 01, 2025
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (13)

R

Riqing Ding

State Key Lab of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Functional and Intelligent Hybrid Materials and Devices, South China Advanced Institute for Soft Matter Science and Technology, School of Emergent Soft Matter South China University of Technology Guangzhou 510640 P.R. China

X

Xiage Zhang

Y

Yidan Luan

State Key Lab of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Functional and Intelligent Hybrid Materials and Devices, South China Advanced Institute for Soft Matter Science and Technology, School of Emergent Soft Matter South China University of Technology Guangzhou 510640 P.R. China

M

Meishan Peng

State Key Lab of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Functional and Intelligent Hybrid Materials and Devices, South China Advanced Institute for Soft Matter Science and Technology, School of Emergent Soft Matter South China University of Technology Guangzhou 510640 P.R. China

W

Wantao Chen

State Key Lab of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Functional and Intelligent Hybrid Materials and Devices, South China Advanced Institute for Soft Matter Science and Technology, School of Emergent Soft Matter South China University of Technology Guangzhou 510640 P.R. China

S

Sijing Wang

S

Shengyao Su

S

Shunyang Lu

State Key Lab of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Functional and Intelligent Hybrid Materials and Devices, South China Advanced Institute for Soft Matter Science and Technology, School of Emergent Soft Matter South China University of Technology Guangzhou 510640 P.R. China

S

Sang Young Jeong

Department of Chemistry, Korea University, Anamro 145, Seoul 02841, Republic of Korea

H

Han Young Woo

X

Xugang Guo

Department of Materials Science and Engineering

K

Kui Feng

Department of Materials Science and Engineering

Z

Zi‐Hao Guo

State Key Lab of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Functional and Intelligent Hybrid Materials and Devices, South China Advanced Institute for Soft Matter Science and Technology, School of Emergent Soft Matter South China University of Technology Guangzhou 510640 P.R. China