Reversible Exfoliation‐Aggregation Dynamics in Ionic COFs for Tunable Interfacial Catalysis
6 affiliations
- 1State Key Laboratory of Applied Organic Chemistry Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province College of Chemistry and Chemical Engineering Lanzhou University Lanzhou People's Republic of China
- 2School of Materials Science and Engineering Key Laboratory of Automobile Materials of MOE Jilin University Changchun People's Republic of China
- 3State Key Laboratory of Supramolecular Structure and Materials College of Chemistry Jilin University Changchun People's Republic of China
- 4School of Chemistry and Chemical Engineering Guangxi Minzu University Nanning People's Republic of China
- 5Guangxi Key Laboratory of Al‐Driven Zero‐Carbon Technology Key Laboratory of New Low‐Carbon Green Chemical Technology Education Department of Guangxi Zhuang Autonomous Region School of Chemistry and Chemical Engineering Guangxi University Nanning People's Republic of China
- 6Key Laboratory of Comprehensive and Highly Efficient Utilization of Salt Lake Resources Qinghai Institute of Salt Lakes Chinese Academy of Sciences Xining People's Republic of China
Abstract
2D covalent organic frameworks (COFs) have emerged as promising functional materials for catalysis, adsorption, sensing, and energy storage. Their interfacial behavior and surface microenvironment play a decisive role in performance, yet these features are typically considered static or irreversible due to the lack of dynamic structure models. In this study, we report the construction of an ionic COF (iCOF), I‐4, designed through precise tuning of its skeleton and counterions, which uniquely exhibits reversable dynamic exfoliation and aggregation behavior in aqueous environments. This enables bidirectional control over particle size and phase states. Photocatalytic hydrogen evolution (PHE) studies reveal a strong correlation between solution concentration, particle size, and hydrogen production efficiency. Notably, I‐4 achieves a remarkable PHE rate of 190 mmol g−1 h−1 at 35°C. Moreover, the material can be fully precipitated and recovered from solution by simple iodide salt addition, enabling closed‐loop material recycling. Mechanistic analysis based on weak‐force interactions and soft‐hard acid‐base theory provides insight into the dynamic exfoliation process, highlighting the synergistic roles of counterion assembly and framework structure. These findings pave the way for the tailored synthesis of next‐generation dynamic COF materials with reversible interfacial adaptability, offering broad application potential in catalysis, ion transport, and molecular separation.
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BibTeX
@article{yang2026reversible,
title = {{Reversible Exfoliation‐Aggregation Dynamics in Ionic COFs for Tunable Interfacial Catalysis}},
author = {Jilu Yang and Xiaofei Zhang and Yue Li and Yuping Cao and Zhaowei Jia and Bo Li and Haitao Feng and Xiaoqiang Cui and Wenwu Qin},
journal = {Advanced Science},
year = {2026},
month = aug,
doi = {10.1002/advs.77122},
url = {https://doi.org/10.1002/advs.77122},
note = {CC BY 4.0},
}
RIS
TY - JOUR
TI - Reversible Exfoliation‐Aggregation Dynamics in Ionic COFs for Tunable Interfacial Catalysis
AU - Jilu Yang
AU - Xiaofei Zhang
AU - Yue Li
AU - Yuping Cao
AU - Zhaowei Jia
AU - Bo Li
AU - Haitao Feng
AU - Xiaoqiang Cui
AU - Wenwu Qin
PY - 2026
DA - 2026/08/14
JO - Advanced Science
DO - 10.1002/advs.77122
UR - https://doi.org/10.1002/advs.77122
AB - 2D covalent organic frameworks (COFs) have emerged as promising functional materials for catalysis, adsorption, sensing, and energy storage. Their interfacial behavior and surface microenvironment play a decisive role in performance, yet these features are typically considered static or irreversible due to the lack of dynamic structure models. In this study, we report the construction of an ionic COF (iCOF), I‐4, designed through precise tuning of its skeleton and counterions, which uniquely exhibits reversable dynamic exfoliation and aggregation behavior in aqueous environments. This enables bidirectional control over particle size and phase states. Photocatalytic hydrogen evolution (PHE) studies reveal a strong correlation between solution concentration, particle size, and hydrogen production efficiency. Notably, I‐4 achieves a remarkable PHE rate of 190 mmol g−1 h−1 at 35°C. Moreover, the material can be fully precipitated and recovered from solution by simple iodide salt addition, enabling closed‐loop material recycling. Mechanistic analysis based on weak‐force interactions and soft‐hard acid‐base theory provides insight into the dynamic exfoliation process, highlighting the synergistic roles of counterion assembly and framework structure. These findings pave the way for the tailored synthesis of next‐generation dynamic COF materials with reversible interfacial adaptability, offering broad application potential in catalysis, ion transport, and molecular separation.
SN - 2198-3844
ER -