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Controlling Electrode-Electrolyte Interactions to Enhance Capacitance
Jamie W Gittins1, Chloe J Balhatchet1, James Hill1,2
1Yusuf Hamied Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, U.K.
Journal of the American Chemical Society
|April 13, 2026
Summary
Metal-organic frameworks (MOFs) with specific functional groups significantly boost electric double-layer capacitance for energy storage. Deprotonated M-O and M-S groups, especially metal-hydroxy linkages, enhance Li+ ion uptake and performance.
Area of Science:
- Materials Science
- Electrochemistry
- Nanotechnology
Background:
- Improving energy storage device performance requires understanding ion-electrode interactions at the molecular level.
- Conventional carbon electrodes have limitations due to structural disorder and undefined surface chemistry.
- Metal-organic frameworks (MOFs) offer tunable structures for studying fundamental electrochemical processes.
Purpose of the Study:
- To investigate the influence of different functional groups on electric double-layer capacitance in MOFs.
- To elucidate the molecular mechanisms behind enhanced ion adsorption and charge storage.
- To establish a chemically tunable strategy for designing advanced porous electrodes.
Main Methods:
- Fabrication of layered MOF electrodes with varying functional groups.
- Electrochemical characterization of electric double-layer capacitance using alkali metal and tetraethylammonium cations.
- Solid-state nuclear magnetic resonance (NMR) spectroscopy to probe ion binding.
- Molecular simulations to model ion-surface interactions.
- Operando X-ray techniques to investigate structural changes during operation.
Main Results:
- Deprotonated M-O and M-S functional groups in MOFs significantly enhance capacitance with Li+ ions compared to TEA+.
- MOFs with metal-hydroxy linkages show the largest capacity increase, attributed to strong Li-O interactions and charge screening.
- Protonated M-NH groups do not yield similar capacitance enhancements.
- NMR and simulations confirm specific Li+ binding at oxygen-rich sites.
- Operando X-ray data exclude cation intercalation as a mechanism.
Conclusions:
- Surface functionalization of MOFs provides a powerful strategy for tuning electric double-layer capacitance.
- Specific ion-surface interactions, particularly Li-O bonding, are key to enhancing charge storage.
- MOFs serve as excellent model systems for understanding fundamental electrochemical principles in porous materials.
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