Multidimensional Modulation via Tailored Covalent Organic Frameworks Enables Stable Inverted Perovskite Solar Cells with 26.21% Efficiency

T Tianzhou Yin (Guangzhou Key Laboratory of Low‐Dimensional Materials and Energy Storage Devices, Collaborative Innovation Center of Advanced Energy Materials, School of Materials and Energy Guangdong University of Technology Guangzhou 510006 P. R. China) Z Zimin Zhang H Hualin Wu (Guangzhou Key Laboratory of Low‐Dimensional Materials and Energy Storage Devices, Collaborative Innovation Center of Advanced Energy Materials, School of Materials and Energy Guangdong University of Technology Guangzhou 510006 P. R. China) H Haiting Tan (Guangzhou Key Laboratory of Low‐Dimensional Materials and Energy Storage Devices, Collaborative Innovation Center of Advanced Energy Materials, School of Materials and Energy Guangdong University of Technology Guangzhou 510006 P. R. China) H Haoxin Wen (Guangzhou Key Laboratory of Low‐Dimensional Materials and Energy Storage Devices, Collaborative Innovation Center of Advanced Energy Materials, School of Materials and Energy Guangdong University of Technology Guangzhou 510006 P. R. China) G Gangsheng Zhou (Guangzhou Key Laboratory of Low‐Dimensional Materials and Energy Storage Devices, Collaborative Innovation Center of Advanced Energy Materials, School of Materials and Energy Guangdong University of Technology Guangzhou 510006 P. R. China) H Hao Li X Xijie Qiu (Guangzhou Key Laboratory of Low‐Dimensional Materials and Energy Storage Devices, Collaborative Innovation Center of Advanced Energy Materials, School of Materials and Energy Guangdong University of Technology Guangzhou 510006 P. R. China) Y Yixuan Guo C Chuangping Liu (Guangzhou Key Laboratory of Low‐Dimensional Materials and Energy Storage Devices, Collaborative Innovation Center of Advanced Energy Materials, School of Materials and Energy Guangdong University of Technology Guangzhou 510006 P. R. China) Z Zhuo Kang (Academy for Advanced Interdisciplinary Science and Technology, Beijing Key Laboratory for Advanced Energy Materials and Technologies, State Key Laboratory for Advanced Metals and Materials) S Shaoming Huang (School of Materials and Energy Guangzhou Key Laboratory of Low‐Dimensional Materials and Energy Storage Devices Guangdong University of Technology Guangzhou Guangdong People's Republic of China)

Abstract

AbstractDespite the remarkable advancements in inverted perovskite solar cells, their commercialization remains hindered by critical bottlenecks in efficiency and stability stemming from inadequate crystallization and unfavorable interfacial states. Herein, for the first time, a judiciously designed hydrazine‐linked covalent organic framework (COF) with long alkane phosphate branch chains, named 12‐SD‐COF, is synthesized and integrated into the perovskite precursor to achieve multidimensional regulation of crystallization, defect states, and charge separation synergistically. It is found that the 12‐SD‐COF featuring periodic pores, large planar structure, and abundant binding groups is extruded from the precursor solution onto the buried interface, surface, and grain boundaries, facilitating oriented crystallization while eliminating defects of perovskites, thereby yielding high‐quality crystals with suppressed non‐radiative recombination. Simultaneously, the interfacial charge separation is synergistically facilitated by the p‐type doping‐optimized energy level alignment and the induced intramolecular electric field, ultimately achieving an exceptional power conversion efficiency (PCE) of 26.21%, the highest yet reported for COF‐modified. Impressively, the non‐encapsulated resultant device delivers greatly improved stabilities, with maintaining over 92% of initial PCE after being aged under 85 °C continuous heating stress for 800 h, 1000 h in 50±3% relative humidity air, and 1200 h under continuous 1‐sun illumination, respectively.

Article Details

Volume / Issue Vol. 37, Issue 29
Published July 01, 2025
ISSN 0935-9648
Publisher Unknown Publisher

Journal Info

Advanced Materials

Unknown Publisher

ISSN: 0935-9648 Physical Sciences

Authors (12)

T

Tianzhou Yin

Guangzhou Key Laboratory of Low‐Dimensional Materials and Energy Storage Devices, Collaborative Innovation Center of Advanced Energy Materials, School of Materials and Energy Guangdong University of Technology Guangzhou 510006 P. R. China

Z

Zimin Zhang

H

Hualin Wu

Guangzhou Key Laboratory of Low‐Dimensional Materials and Energy Storage Devices, Collaborative Innovation Center of Advanced Energy Materials, School of Materials and Energy Guangdong University of Technology Guangzhou 510006 P. R. China

H

Haiting Tan

Guangzhou Key Laboratory of Low‐Dimensional Materials and Energy Storage Devices, Collaborative Innovation Center of Advanced Energy Materials, School of Materials and Energy Guangdong University of Technology Guangzhou 510006 P. R. China

H

Haoxin Wen

Guangzhou Key Laboratory of Low‐Dimensional Materials and Energy Storage Devices, Collaborative Innovation Center of Advanced Energy Materials, School of Materials and Energy Guangdong University of Technology Guangzhou 510006 P. R. China

G

Gangsheng Zhou

Guangzhou Key Laboratory of Low‐Dimensional Materials and Energy Storage Devices, Collaborative Innovation Center of Advanced Energy Materials, School of Materials and Energy Guangdong University of Technology Guangzhou 510006 P. R. China

H

Hao Li

X

Xijie Qiu

Guangzhou Key Laboratory of Low‐Dimensional Materials and Energy Storage Devices, Collaborative Innovation Center of Advanced Energy Materials, School of Materials and Energy Guangdong University of Technology Guangzhou 510006 P. R. China

Y

Yixuan Guo

C

Chuangping Liu

Guangzhou Key Laboratory of Low‐Dimensional Materials and Energy Storage Devices, Collaborative Innovation Center of Advanced Energy Materials, School of Materials and Energy Guangdong University of Technology Guangzhou 510006 P. R. China

Z

Zhuo Kang

Academy for Advanced Interdisciplinary Science and Technology, Beijing Key Laboratory for Advanced Energy Materials and Technologies, State Key Laboratory for Advanced Metals and Materials

S

Shaoming Huang

School of Materials and Energy Guangzhou Key Laboratory of Low‐Dimensional Materials and Energy Storage Devices Guangdong University of Technology Guangzhou Guangdong People's Republic of China