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Updated: May 27, 2025

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High-Connectivity 3D Covalent Organic Frameworks with pdp Net for Efficient C2H2/CO2 Separation.

Jie Zhang1, Haorui Zheng1, Fengqian Chen1

  • 1State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, Department of Chemistry, Jilin University, Changchun, 130012, P. R. China.

Angewandte Chemie (International Ed. in English)
|February 18, 2025
PubMed
Summary

Two new 3D covalent organic frameworks (COFs) with unique cages were synthesized. These advanced COFs demonstrate exceptional capabilities for separating acetylene from carbon dioxide, even in humid conditions.

Keywords:
C2H2/CO2 separationcovalent organic frameworksporous materialsreticular chemistry

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Area of Science:

  • Materials Science
  • Chemistry

Background:

  • High-connectivity 3D covalent organic frameworks (COFs) are promising for various applications due to their complex structures and stability.
  • Synthesizing 3D COFs using mixed high-nodal building units presents a significant challenge in materials chemistry.

Purpose of the Study:

  • To introduce novel 3D COFs, JUC-661 and JUC-662, synthesized from mixed high-nodal building units.
  • To investigate the gas separation capabilities of these new COFs, particularly for acetylene/carbon dioxide mixtures.

Main Methods:

  • Synthesis of two novel 3D COFs (JUC-661 and JUC-662) using D2h-symmetric 8-nodal and D3h-symmetric 6-nodal building blocks.
  • Characterization of the COFs' structure, including unprecedented [8+6]-c pdp nets and mesoporous polyhedral cages.
  • Evaluation of gas adsorption and separation performance using dynamic breakthrough experiments under various humidity conditions.
  • Computational analysis using Monte Carlo simulations and DFT calculations to understand adsorption mechanisms.

Main Results:

  • Successful synthesis of JUC-661 and JUC-662, featuring rare mesoporous polyhedral cages (~3.9 nm).
  • Demonstrated outstanding adsorption selectivities for C2H2/CO2 mixtures (4.3 for JUC-661, 5.9 for JUC-662).
  • Maintained high separation performance under 100% humidity conditions.
  • Computational studies revealed pore cavity structure and fluorination effects enhance C2H2 selectivity.

Conclusions:

  • The study expands the structural diversity of 3D covalent organic frameworks.
  • JUC-661 and JUC-662 show significant potential for energy-efficient gas separation processes.
  • Fluorination of building units can be a strategy to enhance selective adsorption in COFs.