Volume 63, Issue 51 e202411753
Research Article

Construction of Highly Porous and Robust Hydrogen-Bonded Organic Framework for High-Capacity Clean Energy Gas Storage

Jia-Xin Wang

Jia-Xin Wang

State Key Laboratory of Silicon and Advanced Semiconductor Materials School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027 China

These authors contributed equally to this work.

Search for more papers by this author
Prof. Xu Zhang

Prof. Xu Zhang

Jiangsu Engineering Laboratory for Environmental Functional Materials School of Chemistry and Chemical Engineering, Huaiyin Normal University, Huaian, 223300 China

These authors contributed equally to this work.

Search for more papers by this author
Chenghao Jiang

Chenghao Jiang

State Key Laboratory of Silicon and Advanced Semiconductor Materials School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027 China

Search for more papers by this author
Teng-Fei Zhang

Teng-Fei Zhang

State Key Laboratory of Silicon and Advanced Semiconductor Materials School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027 China

Search for more papers by this author
Jiyan Pei

Jiyan Pei

State Key Laboratory of Silicon and Advanced Semiconductor Materials School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027 China

Search for more papers by this author
Dr. Wei Zhou

Dr. Wei Zhou

NIST Center for Neutron Research, National Institute of Standards and Technology, Gaithersburg, MD 20899–6102 USA

Search for more papers by this author
Dr. Taner Yildirim

Dr. Taner Yildirim

NIST Center for Neutron Research, National Institute of Standards and Technology, Gaithersburg, MD 20899–6102 USA

Search for more papers by this author
Prof. Banglin Chen

Corresponding Author

Prof. Banglin Chen

Fujian Provincial Key Laboratory of Polymer Materials College of Chemistry & Materials Science, Fujian Normal University, Fuzhou, 350007 China

Key Laboratory of the Ministry of Education for Advanced Catalysis Materials College of Chemistry and Materials Science, Zhejiang Normal University, Jinhua, 321004 China

Search for more papers by this author
Prof. Guodong Qian

Prof. Guodong Qian

State Key Laboratory of Silicon and Advanced Semiconductor Materials School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027 China

Search for more papers by this author
Prof. Bin Li

Corresponding Author

Prof. Bin Li

State Key Laboratory of Silicon and Advanced Semiconductor Materials School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027 China

Search for more papers by this author
First published: 13 August 2024
Citations: 15

Graphical Abstract

We herein proposed and demonstrated a strategy of constructing the double-walled framework to target a highly porous and robust HOF material (ZJU-HOF-5a), exhibiting one of the highest gravimetric and volumetric surface areas for extraordinary high-pressure methane and hydrogen storage capacities.

Abstract

Development of highly porous and robust hydrogen-bonded organic frameworks (HOFs) for high-pressure methane and hydrogen storage remains a grand challenge due to the fragile nature of hydrogen bonds. Herein, we report a strategy of constructing the double-walled framework to target highly porous and robust HOF (ZJU-HOF-5a) for extraordinary CH4 and H2 storage. ZJU-HOF-5a features a minimized twofold interpenetration with double-walled structure, in which multiple supramolecular interactions are existed between the interpenetrated walls. This structural configuration can notably enhance the framework robustness while maintaining its high porosity, affording one of the highest gravimetric and volumetric surface areas of 3102 m2 g−1 and 1976 m2 cm−3 among the reported HOFs so far. ZJU-HOF-5a thus exhibits an extremely high volumetric H2 uptake of 43.6 g L−1 at 77 K/100 bar and working capacity of 41.3 g L−1 under combined swing conditions (77 K/100 bar→160 K/5 bar), and also impressive methane storage performance with a 5–100 bar working capacity of 187 (or 159) cm3 (STP) cm−3 at 270 K (or 296 K), outperforming most of the reported porous organic materials. Single-crystal X-ray diffraction studies on CH4-loaded ZJU-HOF-5a reveal that abundant supramolecular binding sites combined with ultrahigh porosities account for its high CH4 storage capacities. Combined with high stability, super-hydrophobicity, and easy recovery, ZJU-HOF-5a is placed among the most promising materials for H2 and CH4 storage applications.

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 supplementary material of this article.

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