Enabling Rotated Stacking Displacement in Two‐Dimensional Covalent Organic Frameworks via Interlayer Electrostatic Repulsion

X Xinkun Ma (School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, 21 Nanyang Link, Singapore 637371, Singapore) W Wang‐Kang Han (Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering Jiangnan University Wuxi China) H Haishan Zhu (Institute of Microstructure and Property of Advanced Materials College of Material Science and Engineering Beijing University of Technology Beijing China) T Ting He (Division of Thyroid Surgery, Department of General Surgery and Laboratory of Thyroid and Parathyroid Disease, Frontiers Science Center for Disease-related Molecular Network, West China Hospital, Sichuan University) Z Zhifang Wang (Department of Chemistry, Institute of Molecular Aggregation Science, School of Science) W Wei Zhou X Xue‐Song Wu (School of Chemistry Chemical Engineering and Biotechnology Nanyang Technological University Singapore Singapore) Y Yunxiang Ma Z Ziyue Huang (School of Chemistry Chemical Engineering and Biotechnology Nanyang Technological University Singapore Singapore) Y Yue Zhao J Jingyu Zhang (East China University of Science and Technology , , ,) C Chunqiang Zhuang (Institute of Microstructure and Property of Advanced Materials College of Material Science and Engineering Beijing University of Technology Beijing China) Y Yanli Zhao (School of Chemistry, Chemical Engineering and Biotechnology)

Abstract

ABSTRACT Tuning the interlayer stacking in 2D covalent organic frameworks (2D COFs) allows unique structural and optoelectronic properties. However, the diversity of 2D COF stacking modes is limited to eclipsed, serrated, and shifted stacking. In this study, we develop a method for constructing COFs with rotated stacking by modulating interlayer electrostatic repulsion. COFs with rotated or eclipsed (AA) stacking are obtained via reactions between triamine and dialdehyde monomers with or without pyridinium substituents. Importantly, the modulation of pyridinium substituents enables the transformation of different stacking modes, as well as the conversion of amorphous to crystalline materials. Moreover, multicomponent‐based stacking regulation strategies are found to efficiently mediate photocatalytic hydrogen peroxide production, owing to their tunable photophysical properties. Our findings provide perspectives on leveraging interlayer repulsion to tailor interlayer stacking in 2D COFs, thereby diversifying their topologies and improving their optoelectronic properties.

Article Details

Volume / Issue Vol. 65, Issue 11
Published March 09, 2026
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (13)

X

Xinkun Ma

School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, 21 Nanyang Link, Singapore 637371, Singapore

W

Wang‐Kang Han

Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering Jiangnan University Wuxi China

H

Haishan Zhu

Institute of Microstructure and Property of Advanced Materials College of Material Science and Engineering Beijing University of Technology Beijing China

T

Ting He

Division of Thyroid Surgery, Department of General Surgery and Laboratory of Thyroid and Parathyroid Disease, Frontiers Science Center for Disease-related Molecular Network, West China Hospital, Sichuan University

Z

Zhifang Wang

Department of Chemistry, Institute of Molecular Aggregation Science, School of Science

W

Wei Zhou

X

Xue‐Song Wu

School of Chemistry Chemical Engineering and Biotechnology Nanyang Technological University Singapore Singapore

Y

Yunxiang Ma

Z

Ziyue Huang

School of Chemistry Chemical Engineering and Biotechnology Nanyang Technological University Singapore Singapore

Y

Yue Zhao

J

Jingyu Zhang

East China University of Science and Technology , , ,

C

Chunqiang Zhuang

Institute of Microstructure and Property of Advanced Materials College of Material Science and Engineering Beijing University of Technology Beijing China

Y

Yanli Zhao

School of Chemistry, Chemical Engineering and Biotechnology