Precise Structure Regulation Induced Morphological Ordering Enables All‐Polymer Solar Cells With 20.29% Efficiency and Extreme Mechanical Robustness

H Huanhuan Gao L Lingya Sun (Shandong Provincial Key Laboratory for Science of Material Creation and Energy Conversion Science Center for Material Creation and Energy Conversion Institute of Frontier Chemistry School of Chemistry and Chemical Engineering Shandong University Qingdao China) Y Yanna Sun L Lei Wang X Xiao Ma (State Key Laboratory of Solidification Processing) M Meiyuan Zu (Qingdao Innovation and Development Center Harbin Engineering University Qingdao China) X Xianshao Zou (Qingdao Innovation and Development Center, Harbin Engineering University 4 , Qingdao 266000,) Y Yuanyuan Kan (Shandong Provincial Key Laboratory for Science of Material Creation and Energy Conversion Science Center for Material Creation and Energy Conversion Institute of Frontier Chemistry School of Chemistry and Chemical Engineering Shandong University Qingdao China) X Xunchang Wang (Key Laboratory of Optoelectronic Chemical Materials and Devices (Ministry of Education) School of Optoelectronic Materials & Technology Jianghan University Wuhan China) R Renqiang Yang X Xiangjian Wan (State Key Laboratory and Institute of Elemento-Organic Chemistry, The Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer Materials, Renewable Energy Conversion and Storage Center (RECAST), Frontiers Science Center for New Organic Matter, College of Chemistry) Y Yiyu Feng (School of Materials Science and Engineering Shandong Key Laboratory of Functional‐Structural Integrated Ceramics Discipline and Technology Center for High Temperature Functional Ceramics Shandong University of Technology Zibo China) K Ke Gao (State Key Laboratory of Bioactive Substance and Function of Natural Medicines, CAMS Key Laboratory of Enzyme and Biocatalysis of Natural Drugs, and NHC Key Laboratory of Biosynthesis of Natural Products) Y Yongsheng Chen (Department of Neurosurgery The Tenth Affiliated Hospital Southern Medical University Dongguan China)

Abstract

ABSTRACT All polymer organic solar cells (APSCs) demonstrate distinctive advantages in balancing device efficiency while enhancing operational stability, particularly regarding mechanical robustness. However, their power conversion efficiency (PCE) has long been behind that of the corresponding devices with small molecular acceptors. This is due to the precise chemical structure modulation of polymer acceptors (PAs), enabling relatively coplanar conformation and ordered molecular stacking and thus achieving ideal morphology, which remains critically challenging. Herein, in this work, we have designed two biaxial conjugate extension PAs, with various side chain/terminal substituents to control their intermolecular non‐covalent interactions, thereby optimizing aggregation behavior and microstructural orientation of polymer assemblies. It was found that the alkoxy‐functionalized PQxO‐IT facilitates stronger intermolecular interactions and tighter π‐π stacking. Furthermore, the PQx‐FT:PQxO‐IT composite promoted charge carrier mobility and charge transport, while effectively suppressing non‐radiative decay pathways. Consequently, the corresponding ternary device achieved the highest PCE of 20.29% (certified as 20.03%) for the APSC systems so far. Furthermore, the tight and ordered molecular packing endowed the flexible device with a PCE of 18.93% and remarkable durability during continuous bending tests. This study demonstrates a precise structure modulation strategy that offers a viable materials design pathway for high‐performance flexible photovoltaics.

Article Details

Volume / Issue Vol. 65, Issue 32
Published August 03, 2026
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (14)

H

Huanhuan Gao

L

Lingya Sun

Shandong Provincial Key Laboratory for Science of Material Creation and Energy Conversion Science Center for Material Creation and Energy Conversion Institute of Frontier Chemistry School of Chemistry and Chemical Engineering Shandong University Qingdao China

Y

Yanna Sun

L

Lei Wang

X

Xiao Ma

State Key Laboratory of Solidification Processing

M

Meiyuan Zu

Qingdao Innovation and Development Center Harbin Engineering University Qingdao China

X

Xianshao Zou

Qingdao Innovation and Development Center, Harbin Engineering University 4 , Qingdao 266000,

Y

Yuanyuan Kan

Shandong Provincial Key Laboratory for Science of Material Creation and Energy Conversion Science Center for Material Creation and Energy Conversion Institute of Frontier Chemistry School of Chemistry and Chemical Engineering Shandong University Qingdao China

X

Xunchang Wang

Key Laboratory of Optoelectronic Chemical Materials and Devices (Ministry of Education) School of Optoelectronic Materials & Technology Jianghan University Wuhan China

R

Renqiang Yang

X

Xiangjian Wan

State Key Laboratory and Institute of Elemento-Organic Chemistry, The Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer Materials, Renewable Energy Conversion and Storage Center (RECAST), Frontiers Science Center for New Organic Matter, College of Chemistry

Y

Yiyu Feng

School of Materials Science and Engineering Shandong Key Laboratory of Functional‐Structural Integrated Ceramics Discipline and Technology Center for High Temperature Functional Ceramics Shandong University of Technology Zibo China

K

Ke Gao

State Key Laboratory of Bioactive Substance and Function of Natural Medicines, CAMS Key Laboratory of Enzyme and Biocatalysis of Natural Drugs, and NHC Key Laboratory of Biosynthesis of Natural Products

Y

Yongsheng Chen

Department of Neurosurgery The Tenth Affiliated Hospital Southern Medical University Dongguan China