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Radiation-Assisted Synthesis of Crown Ether-Modified Covalent Organic Frameworks for Lithium Isotope Separation
Summary:
The authors from Peking University and other institutions: developed a crown ether-modified covalent organic framework (COF) material using γ-ray radiation-assisted synthesis, achieving high lithium adsorption capacity and effective 6Li/7Li isotope separation.
Background:
1. Previous researchers have explored various methods for lithium isotope separation, including physical and chemical techniques, but challenges remain in terms of efficiency, environmental impact, and ease of recycling.
2. The authors proposed an innovative method of radiation-assisted synthesis to immobilize crown ethers onto COFs, aiming to enhance lithium adsorption and separation performance.
Research Content:
1. Synthesis:
The authors synthesized a series of crown ether-modified COFs ([15C5]n%-(TzDa-G-x%)) using γ-ray radiation-induced grafting of glycidyl methacrylate (GMA) followed by chemical modification with 4-aminobenzo-15-crown-5.
2. Characterizations:
1) The specific surface area of [15C5]57%-(TzDa-G-50%) was 222 m²/g, indicating good porosity.
2) SEM/TEM tests showed that the material had a fibrous morphology before grafting and a coral-like morphology after grafting and immobilization.
3) ATR-FTIR, XPS, and solid-state 13C NMR confirmed successful grafting of GMA and immobilization of crown ether.
3. Application:
The material was tested for lithium adsorption and 6Li/7Li isotope separation. It exhibited fast adsorption kinetics, achieving a capacity of 3.6 mg/g within 30 min and a saturation capacity of 7.3 mg/g in acetonitrile. The single-stage separation factor was 1.014 ± 0.001. Dynamic adsorption column experiments showed stable performance over four cycles with a Li+ removal rate of over 99%.
4. Mechanism:
The analysis of experimental results indicated that the presence of crown ether groups facilitated lithium adsorption and separation. Theoretical calculations and experimental data suggested that the optimal immobilization yield and crystallinity of the COF were crucial for achieving high performance.
Outlook:
This research demonstrates the potential of radiation-assisted synthesis for creating functional COFs with high lithium adsorption capacity and effective isotope separation, offering new opportunities for developing advanced materials for nuclear applications.
Radiation-Assisted Synthesis of Crown Ether-Modified Covalent Organic Frameworks for Lithium Isotope Separation
Authors: Shouchao Zhong, Yue Wang, Jianhui Lan, Mingshu Xie, Yiqian Wu, Jiuqiang Li, Fujian Liu, Lilong Jiang, Jing Peng, Liyong Yuan, Maolin Zhai, Weiqun Shi
DOI: 10.31635/ccschem.024.202303787
Link: https://doi.org/10.31635/ccschem.024.202303787
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