Crystalline Lithium Imidazolate Covalent Organic Frameworks with High Li-Ion Conductivity
Yiming Hu1, Nathan Dunlap2, Shun Wan3
1Department of Chemistry , University of Colorado , Boulder , Colorado 80309 , United States.
Journal of the American Chemical Society
|April 16, 2019
Summary
Researchers developed new imidazolate-containing ionic covalent organic frameworks (ICOFs) for solid-state electrolytes. These ICOFs exhibit high lithium-ion conductivity and low activation energy, paving the way for advanced solid-state batteries.
Area of Science:
- Materials Science
- Electrochemistry
- Polymer Chemistry
Background:
- Ionic covalent organic frameworks (ICOFs) are emerging as advanced materials for solid-state electrolytes.
- Developing efficient solid-state electrolytes is crucial for next-generation energy storage devices.
Purpose of the Study:
- To report the first series of crystalline imidazolate-containing ICOFs as single-ion conducting solid electrolyte materials.
- To investigate the structure-property relationships influencing ion conductivity in these ICOFs.
Main Methods:
- Synthesis of crystalline imidazolate-containing ICOFs.
- Characterization of ICOF structures and porous frameworks.
- Measurement of ionic conductivity and activation energy for lithium-ion transport.
Main Results:
- Achieved high ionic conductivity (up to 7.2 × 10-3 S cm-1) and low activation energy (0.10 eV).
- Demonstrated that weak Li ion-imidazolate binding and well-defined porous structures enhance ion transport.
- Found that electron-withdrawing substituents significantly improve ion conductivity by weakening ion-pair interactions.
Conclusions:
- Imidazolate-containing ICOFs represent a novel class of highly efficient single-ion conducting solid electrolytes.
- These ICOFs offer a promising bottom-up approach for developing materials for all-solid-state electrolytic devices.
- Tailoring substituent electronic properties is an effective strategy to optimize ion conductivity in ICOFs.
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