期刊
ACS APPLIED MATERIALS & INTERFACES
卷 9, 期 39, 页码 33802-33809出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.7b08414
关键词
sodium-ion batteries; electrolytes; hard carbon; passivation; high concentration
资金
- ESICB project
- amp
- quot
- Priority Issue on Post K Computeramp
- quot
- of MEXT [5]
- quot
- Materials Research by Information Integrationquot
- Initiative (MT2I) project at JST
- Japan Society for the Promotion of Science [16F16051]
- [hp160075]
- [hp160080]
- [hp160225]
- Grants-in-Aid for Scientific Research [16F16051] Funding Source: KAKEN
The passivation of negative electrodes is key to achieving prolonged charge-discharge cycling with Na-ion batteries. Here, we report the unusual passivation ability of superconcentrated Na-salt electrolytes. For example, a 50 mol % sodium bis(fluorosulfonyl)amide (NaFSA)/succinonitrile (SN) electrolyte enables highly reversible Na+ insertion into a hard carbon negative electrode without any electrolyte additive, functional binder, or electrode pretreatment. Importantly, an anion-derived passivation film is formed via preferential reduction of the anion upon charging, which can effectively suppress further electrolyte reduction. As a structural characteristic of the electrolyte, most anions are coordinated to multiple Na+ cations at high concentration, which shifts the lowest unoccupied molecular orbitals of the anions downward, resulting in preferential anion reduction. The present work provides a new understanding of the passivation mechanism with respect to the coordination state of the anion.
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