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A Needle in a Haystack: Transient Porosity in a Closed Pore Square Lattice Coordination Network
Kyriaki Koupepidou1, Alan C Eaby1, Debobroto Sensharma1
1Bernal Institute, Department of Chemical Sciences, University of Limerick, Limerick, V94 T9PX, Ireland.
Angewandte Chemie (International Ed. in English)
|January 21, 2025
Summary
This study reveals how gases move through closed pores in crystalline solids using a novel coordination network. The material selectively adsorbs acetylene over carbon dioxide, suggesting potential for gas separation applications.
Area of Science:
- Materials Science
- Chemistry
- Crystallography
Background:
- Understanding guest transport through discrete voids in crystalline solids is challenging.
- Coordination networks offer tunable structures for gas sorption studies.
- The role of linker flexibility in guest diffusion remains an active research area.
Purpose of the Study:
- To investigate the gas sorption properties of a nonporous coordination network, {[Co(bib)2Cl2]·2MeOH}n (sql-bib-Co-Cl-α).
- To elucidate the guest transport mechanism through closed pores via gate-opening.
- To explore the potential of this material for selective gas adsorption and separation.
Main Methods:
- Synthesis and characterization of {[Co(bib)2Cl2]·2MeOH}n (sql-bib-Co-Cl-α).
- Single-crystal to single-crystal (SC-SC) phase transformations monitored by Powder X-ray Diffraction (PXRD).
- Gas sorption experiments (C2H2, CO2) at different temperatures and pressures.
- In situ Differential Scanning Calorimetry (DSC) and in situ Single-Crystal X-ray Diffraction (SCXRD).
- Computational studies to understand guest transport mechanisms.
Main Results:
- A coordination network with square lattice (sql) topology and a flexible 1,3-bis(1H-imidazol-1-yl)benzene (bib) linker was synthesized.
- SC-SC transformations led to phases with accessible closed pores (sql-bib-Co-Cl-β) after desolvation and activation.
- sql-bib-Co-Cl-β exhibited preferential adsorption of acetylene (C2H2) over carbon dioxide (CO2) via gate-opening mechanisms at specific pressures.
- The flexible bib ligand was identified as crucial for the guest transport mechanism.
Conclusions:
- The study demonstrates guest transport through gate-opening mechanisms in a crystalline solid with transiently accessible pores.
- The coordination network shows selective adsorption of C2H2 over CO2, highlighting its potential for gas separations.
- The angular and flexible nature of the bib linker plays a key role in controlling guest access and transport.
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