Journal
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
Volume 166, Issue 13, Pages A3051-A3058Publisher
ELECTROCHEMICAL SOC INC
DOI: 10.1149/2.1201913jes
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Funding
- U.S. Department of Energy (DOE) [DE-AC36-08GO28308]
- National Renewable Energy Laboratory's Laboratory Directed Research and Development Program
- Energy Frontier Research in Extreme Environments (EFree) Center, an Energy Frontier Research Center - US Department of Energy, Office of Science [DE-SC0001057]
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The development of advanced anodes for low-cost room temperature sodium-ion batteries (SIBs) with high cycling stability is of great significance. Silicon clathrates are promising intercalation anodes due to their cage-like frameworks. It is predicted that the open cages can easily accommodate alkali ions with negligible volume changes. However, the complicated surface structure and chemical reactions make it challenging to understand the electrochemical performance of clathrate anodes in SIBs. In this paper, we evaluated the performance of type II clathrate anodes in SIBs. A slightly elevated testing temperature (45 degrees C) is shown to improve the cell capacity and rate performance due to the improved ionic conductivity. However, side reactions on the solid electrolyte interface (SEI) and loss of active material during the first sodiation process contribute to the low Coulombic efficiency during the first cycle. Analysis is supported by electrode morphology, elemental mapping, and X-ray photoelectron spectroscopy (XPS) on the clathrate electrodes at different electrochemical states. Na+ ion transport behavior between clathrate cages and surface in terms of migration barriers was also computed to explain the positive effect of higher cell testing temperature, and the low Coulombic efficiency of the first cycle. (C) The Author(s) 2019. Published by ECS.
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