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Hard Carbon Structural Engineering Enables Sodium Cluster Capture with Enhanced Adsorption-Insertion-Filling Storage
Qiaofeng Huang1, Yuan Xu1, Keming Song2
1School of Chemistry, South China Normal University, Guangzhou 510006, China.
Hard carbon electrodes achieve higher sodium-ion battery energy density by optimizing low-potential plateau capacity. Mesoporous structures enhance sodium storage via quasi-metallic clusters in closed pores, boosting capacity by 82.5%.
Area of Science:
- Materials Science
- Electrochemistry
- Energy Storage
Background:
- Enhancing sodium-ion battery energy density requires improving hard carbon (HC) negative electrodes' low-potential plateau capacity.
- The microstructural origins of sodium storage in HC's low-potential region are not fully understood due to structural complexity.
Purpose of the Study:
- To establish a direct correlation between HC microstructure and electrochemical behavior for sodium storage.
- To elucidate the mechanism of sodium storage in the low-potential region of HC electrodes.
- To guide the rational design of high-performance HC negative electrodes.
Main Methods:
- Direct correlation of microstructure and electrochemical behavior.
- In situ electrochemical impedance spectroscopy (EIS) with relaxation time distribution analysis.
- In situ Raman spectroscopy combined with multimodal structural characterizations.
Main Results:
- Sodium storage occurs via quasi-metallic Na+ clusters in closed pores, regulated by mesoporous architectures.
- Mesoporous structures enhance plateau capacity by 82.5% and initial discharge capacity from 168.4 to 347.7 mAh g−1 compared to microporous structures.
- Irreversible solid electrolyte interphase evolution stabilizes interfacial kinetics; a multistep 'adsorption-intercalation/filling' mechanism is verified.
Conclusions:
- Surface mesoporous structures are crucial for activating plateau capacity and facilitating efficient Na+ diffusion in HC electrodes.
- Understanding the role of pore structures provides fundamental insights for designing superior HC negative electrodes.
- This study resolves mechanistic ambiguities, paving the way for advanced sodium-ion battery development.
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