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[Cu(ina)₂] Reverse Separation of CO2 and Acetylene in Two Isostructural Copper-Pyridine-MOFs
Summary:
The authors from Sun Yat-Sen University and Fujian Normal University developed a copper-based metal-organic framework (MOF) material, Cu(ina)₂, with ultramicroporous structures, achieving selective adsorption of acetylene (C₂H₂) over carbon dioxide (CO₂) in gas separation applications.
Background:
1. Separating acetylene from carbon dioxide is crucial in industrial gas purification, but it is highly challenging due to their similar molecular shapes and physical properties. Previous researchers have focused on developing MOFs for gas separation, achieving some success, yet most materials exhibit C₂H₂-selective adsorption, which is not ideal for CO₂ removal.
2. The authors in this study proposed an innovative approach by adjusting the pore structures of isoreticular MOFs to achieve CO₂-selective adsorption, resulting in a reverse separation mechanism that effectively captures CO₂ while allowing pure C₂H₂ to be produced.
Research Content:
1.Synthesis:
The authors synthesized Cu(ina)₂ using a solvothermal method, combining Cu(NO₃)₂·2.5H₂O, isonicotinic acid (Hina), and iodine in water, heated at 140°C for 72 hours, and then cooled to room temperature.
2.Characterizations:
- BET surface area measurements showed a surface area of 230 m²/g for Cu(ina)₂.
- The pore size distribution indicated a pore aperture of 4.1 Å, matching the molecular dimensions of C₂H₂ and CO₂.
- SEM tests revealed the material as black block crystals with irregular bulk particles.
3.Application:
- Gas adsorption experiments demonstrated that Cu(ina)₂ exhibited a C₂H₂/CO₂ selectivity of 3.4 at room temperature, selectively adsorbing C₂H₂ over CO₂.
- Dynamic breakthrough experiments showed that Cu(ina)₂ could produce high-purity C₂H₂ (>99.9%) from a CO₂/C₂H₂ mixture under ambient conditions.
4.Mechanism:
- Neutron powder diffraction experiments confirmed that CO₂ molecules preferentially oriented along the pore channels during adsorption, while C₂H₂ molecules bound in a distorted configuration due to their opposite quadrupole moments.
- Density functional theory (DFT) calculations and Grand Canonical Monte Carlo (GCMC) simulations supported the experimental findings, indicating that the compact pore space of Cu(ina)₂ hindered the adsorption of polarizable C₂H₂, leading to CO₂-selective adsorption.
Outlook:
This research achieved a significant breakthrough in the design of MOFs for gas separation by reversing the selectivity from C₂H₂ to CO₂. The findings provide a new strategy for developing microporous materials with tailored pore structures for efficient gas purification processes.
Reverse Separation of Carbon Dioxide and Acetylene in Two Isostructural Copper Pyridine-Carboxylate Frameworks
Authors: Jing-Hong Li, You-Wei Gan, Jun-Xian Chen, Rui-Biao Lin, Yisi Yang, Hui Wu, Wei Zhou, Banglin Chen, Xiao-Ming Chen
DOI: 10.1002/anie.202400823
Link: https://onlinelibrary.wiley.com/doi/10.1002/anie.202400823
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