Fully Locked Conjugated Backbones in Simple‐Structured Polymer Donors Enabling High‐Performance Organic Solar Cells

G Gening Xie (College of Materials Science and Opto‐Electronic Technology, Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences Beijing 101408 China) J Jiarui Wang (School of Materials Science and Engineering, Nanyang Technological University, 50 Nanyang Avenue, Singapore 639798, Singapore) J Jikai Lv S Sixuan Wang Y YuQi Hou X Xubing Bai Z Ziyang Han (College of Materials Science and Optoelectronic Technology, Center of Materials Science and Optoelectronics Engineering) X Xiaobin Gu (College of Materials Science and Optoelectronic Technology Center of Materials Science and Optoelectronics Engineering, CAS Center for Excellence in Topological Quantum Computation, CAS Key Laboratory of Vacuum Physic) C Congqi Li (College of Materials Science and Optoelectronic Technology, Center of Materials Science and Optoelectronics Engineering, CAS Center for Excellence in Topological Quantum Computation, CAS Key Laboratory of Vacuum Physics) J Jiali Weng M Meng Zhang Z Zheng Tang (Henan Key Laboratory of Polyoxometalate Chemistry, College of Chemistry and Molecular Sciences) Q Qian Peng (State Key Laboratory of Elemento-Organic Chemistry and Tianjin Key Laboratory of Biosensing and Molecular Recognition College of Chemistry, Nankai University, 94 Weijin Road, Tianjin 300071, China) Y Yunhao Cai X Xin Zhang H Hui Huang (Center of Basic Molecular Science (CBMS), Department of Chemistry)

Abstract

Abstract The development of wide‐bandgap polymer donors with cost‐effectiveness is pivotal for advancing the commercialization of organic solar cells (OSCs). However, these materials often suffer from conformational disorder and distortion, due to the presence of multiple rotatable σ‐bonds within their conjugated backbones. This study presents a series of simple‐structured polymer donors PBDT‐TBT‐X (X = H, F, and Cl), and systematically investigates the role of the type and strength of noncovalent conformational locks (NoCLs) in regulating backbone conformations, optoelectronic properties, pre‐aggregation behavior, and charge transport properties. Remarkably, the dual‐locking strategy involving S···O and S···Cl NoCLs achieves the most highly planar conformation with a fully locked backbone. As a result, the binary OSC device based on PBDT‐TBT‐Cl achieves a power conversion efficiency (PCE) of 16.11%, much higher than its PBDT‐TBT‐H (6.35%) and PBDT‐TBT‐F (12.69%) counterparts. Notably, when utilized as a third component, PBDT‐TBT‐Cl enables a ternary OSC device with a PCE exceeding 20%. This work establishes a clear conformation−property−performance relationship, underscoring the critical role of fully locked conformations in designing high‐performance and cost‐effective polymer donors.

Article Details

Volume / Issue Vol. 64, Issue 52
Published December 22, 2025
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (16)

G

Gening Xie

College of Materials Science and Opto‐Electronic Technology, Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences Beijing 101408 China

J

Jiarui Wang

School of Materials Science and Engineering, Nanyang Technological University, 50 Nanyang Avenue, Singapore 639798, Singapore

J

Jikai Lv

S

Sixuan Wang

Y

YuQi Hou

X

Xubing Bai

Z

Ziyang Han

College of Materials Science and Optoelectronic Technology, Center of Materials Science and Optoelectronics Engineering

X

Xiaobin Gu

College of Materials Science and Optoelectronic Technology Center of Materials Science and Optoelectronics Engineering, CAS Center for Excellence in Topological Quantum Computation, CAS Key Laboratory of Vacuum Physic

C

Congqi Li

College of Materials Science and Optoelectronic Technology, Center of Materials Science and Optoelectronics Engineering, CAS Center for Excellence in Topological Quantum Computation, CAS Key Laboratory of Vacuum Physics

J

Jiali Weng

M

Meng Zhang

Z

Zheng Tang

Henan Key Laboratory of Polyoxometalate Chemistry, College of Chemistry and Molecular Sciences

Q

Qian Peng

State Key Laboratory of Elemento-Organic Chemistry and Tianjin Key Laboratory of Biosensing and Molecular Recognition College of Chemistry, Nankai University, 94 Weijin Road, Tianjin 300071, China

Y

Yunhao Cai

X

Xin Zhang

H

Hui Huang

Center of Basic Molecular Science (CBMS), Department of Chemistry