Volume 64, Issue 28 e202500163
Research Article

High-Performance Perovskite Solar Cells via 3D Covalent Organic Frameworks: Enhanced Efficiency Through Precision Interface Engineering

Shanyue Wei

Shanyue Wei

Engineering Research Center of Environment-Friendly Function Materials, Ministry of Education, College of Materials Science & Engineering, Huaqiao University, Xiamen, Fujian Province, 361021 China

CAS Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Provincial Key Laboratory of Nanomaterials, State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian Province, 350002 China

Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials, Xiamen Institute of Rare Earth Materials, Haixi Institutes, Chinese Academy of Sciences, Xiamen, Fujian Province, 361021 China

Both authors contributed equally to this work.

Search for more papers by this author
Weichun Pan

Weichun Pan

Engineering Research Center of Environment-Friendly Function Materials, Ministry of Education, College of Materials Science & Engineering, Huaqiao University, Xiamen, Fujian Province, 361021 China

Both authors contributed equally to this work.

Search for more papers by this author
Jia Liu

Jia Liu

CAS Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Provincial Key Laboratory of Nanomaterials, State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian Province, 350002 China

Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials, Xiamen Institute of Rare Earth Materials, Haixi Institutes, Chinese Academy of Sciences, Xiamen, Fujian Province, 361021 China

Search for more papers by this author
Jihuai Wu

Jihuai Wu

Engineering Research Center of Environment-Friendly Function Materials, Ministry of Education, College of Materials Science & Engineering, Huaqiao University, Xiamen, Fujian Province, 361021 China

Search for more papers by this author
Yiming Xie

Corresponding Author

Yiming Xie

Engineering Research Center of Environment-Friendly Function Materials, Ministry of Education, College of Materials Science & Engineering, Huaqiao University, Xiamen, Fujian Province, 361021 China

CAS Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Provincial Key Laboratory of Nanomaterials, State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian Province, 350002 China

E-mail: [email protected]; [email protected]; [email protected]

Search for more papers by this author
Xiaowei Wu

Corresponding Author

Xiaowei Wu

CAS Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Provincial Key Laboratory of Nanomaterials, State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian Province, 350002 China

Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials, Xiamen Institute of Rare Earth Materials, Haixi Institutes, Chinese Academy of Sciences, Xiamen, Fujian Province, 361021 China

E-mail: [email protected]; [email protected]; [email protected]

Search for more papers by this author
Can-Zhong Lu

Corresponding Author

Can-Zhong Lu

CAS Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Provincial Key Laboratory of Nanomaterials, State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian Province, 350002 China

Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials, Xiamen Institute of Rare Earth Materials, Haixi Institutes, Chinese Academy of Sciences, Xiamen, Fujian Province, 361021 China

University of Chinese Academy of Sciences, Beijing, 100049 China

E-mail: [email protected]; [email protected]; [email protected]

Search for more papers by this author
First published: 29 April 2025
Citations: 1

Graphical Abstract

Two donor-acceptor 3D COFs synthesized via Schiff base reactions were integrated into perovskite solar cells’ SAMs. Their architecture enabled efficient charge separation, stable interfacial anchoring, and optimized energy alignment, enhancing hole transport and perovskite quality and reduced defect density. This achieving PCEs up to 25.20%, demonstrating COFs' potential in advancing PSC efficiency.

Abstract

Covalent organic frameworks (COFs), a class of porous polymers with tunable 2D or 3D structures, have drawn significant attention for their exceptional versatility across various applications. Recently, the integration of COFs into perovskite solar cells (PSCs) has emerged as a promising strategy to address critical challenges, such as instability, interfacial recombination losses, and lead-associated environmental risks. Enhanced charge transport channels, passivation of defects, and customizable molecule architectures are some of the special benefits that COFs offer. In this study, we used Schiff base reactions to create two donor–acceptor (D-A) type COFs with an 8+2 connection motif, which were integrated into PSC self-assembled (SAM) layers. According to characterizations and theoretical calculations, COFs not only effectively optimize the energy level of the ITO/SAM substrate but also passivate perovskite defects and suppress defect-assisted recombination in PSC devices. These modifications significantly enhanced carrier transport and extraction, resulting in an increase in power conversion efficiency (PCE) from 22.57% to 25.20% (DP-BE) and 24.21% (DP-DBE). This work highlights the potential of COFs as multifunctional modifiers for interfacial engineering in PSCs, offering a promising route to improve device performance and stability.

Conflict of Interests

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available in the Supporting Information of this article.

The full text of this article hosted at iucr.org is unavailable due to technical difficulties.