期刊
JOURNAL OF POWER SOURCES
卷 513, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.jpowsour.2021.230554
关键词
Prussian blue; Stability; Dynamic transformation; Sodium-ion battery
资金
- National Natural Science Foundation of China [21422603, U1662120, 21978152]
This work investigates the irreversible transformation of sodium positions in iron hexacyanoferrate during electrochemical cycling, with electron transfer between high spin and low spin iron states contributing to stabilizing the framework. The study focuses on finding an operating window with minimal transformation to achieve high cycling stability for sodium-rich iron hexacyanoferrate.
In this work, sodium-rich iron hexacyanoferrate Na1.74Fe[Fe(CN)6]0.90.2.07H2O (NaFeHCF) with a cubic structure is firstly prepared via a bottom-up approach. The electrochemical reaction mechanism and cycling performance maintenance of as-prepared NaFeHCF are carefully investigated. It is found that there exists some irreversible transformation of sodium positions in iron hexacyanoferrate during electrochemical cycling. Due to the highly itinerant electron state between high spin FeHS and low spin FeLS during redox reaction, the electron transfer in the FeLS3+/FeLS2+ at above 4 V gradually shift to that in the FeHS3+/FeHS2+ at about 3.35 V. However, such a dynamic transformation is not favorable for cycling stability, as more sodium content left in the 24d positions of cubic structure helps stabilize the framework and alleviate the capacity fading. The effects of the cutoff potential, the activated rate at 1st cycle, and the temperature are carefully investigated to find an operating window with insignificant transformation, where the sodium-rich iron hexacyanoferrate presents high cycling stability at 25 degrees C (with a capacity retention of 84.1% for 500 cycles at the current density of 600 mAg-1).
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