期刊
INORGANIC CHEMISTRY
卷 61, 期 28, 页码 10915-10924出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.2c01393
关键词
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资金
- National Natural Science Foundation of China [22090043, 21622101, 22103019]
- Guangxi Natural Science Foundation [2019GXNSFGA245006]
- Guangxi Key Laboratory of Electrochemical and Magneto-chemical Functional Materials [EMFM20211111]
A study on a nonstoichiometric melilite oxide ion conductor showed that interstitial oxide ions in the pentagonal rings can be replaced by confined electron anions, converting the conductor into a zero-dimensional electride. Compared to the framework oxide ions, the interstitial oxide ions are more active and easily reducible, leading to enhanced electronic conductivity.
A nonstoichiometric La1.5Sr0.5Ga3O7.2 5 melilite oxide ion conductor features active interstitial oxygen defects in its pentagonal rings with high mobility. In this study, electron localization function calculated by density functional theory indicated that the interstitial oxide ions located in the pentagonal rings of gallate melilites may be removed and replaced by electron anions that are confined within the pentagonal rings, which would therefore convert the melilite interstitial oxide ion conductor into a zero-dimensional (0D) electride. The more active interstitial oxide ions, compared to the framework oxide ions, make the La(1.5)Sr(0.5)Ga(3)O(7.2 5 )melilite structure more reducible by CaH2 using topotactic reduction, in contrast to the hardly reducible nature of parent LaSrGa3O7. The topotactic reduction enhances the bulk electronic conduction (sigma 0.003 S/cm at 400 ?) by 1 order of magnitude for La1.5Sr0.5Ga3O7.2 5. The oxygen loss in the melilite structure was verified and most likely took place on the active interstitial oxide ions. The identified confinement space for electronic anions in melilite interstitial oxide ion conductors presented here provides a strategy to access inorganic electrides from interstitial oxide ion conductor electrolytes.
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