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Title: Electrochemical Properties and Challenges of Type II Silicon Clathrate Anode in Sodium Ion Batteries

Abstract

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.

Authors:
 [1];  [2];  [2];  [1]; ORCiD logo [1]; ORCiD logo [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  2. Colorado School of Mines, Golden, CO (United States). Dept. of Physics
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE National Renewable Energy Laboratory (NREL), USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1569447
Report Number(s):
NREL/JA-5400-73015
Journal ID: ISSN 0013-4651
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 166; Journal Issue: 13; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; sodium ion batteries; type II silicon clathrate; anode performance assessment

Citation Formats

Li, Xuemin, Steirer, K. Xerxes, Krishna, Lakshmi, Xiao, Chuanxiao, Fink, Kae, and Santhanagopalan, Shriram. Electrochemical Properties and Challenges of Type II Silicon Clathrate Anode in Sodium Ion Batteries. United States: N. p., 2019. Web. doi:10.1149/2.1201913jes.
Li, Xuemin, Steirer, K. Xerxes, Krishna, Lakshmi, Xiao, Chuanxiao, Fink, Kae, & Santhanagopalan, Shriram. Electrochemical Properties and Challenges of Type II Silicon Clathrate Anode in Sodium Ion Batteries. United States. doi:10.1149/2.1201913jes.
Li, Xuemin, Steirer, K. Xerxes, Krishna, Lakshmi, Xiao, Chuanxiao, Fink, Kae, and Santhanagopalan, Shriram. Tue . "Electrochemical Properties and Challenges of Type II Silicon Clathrate Anode in Sodium Ion Batteries". United States. doi:10.1149/2.1201913jes. https://www.osti.gov/servlets/purl/1569447.
@article{osti_1569447,
title = {Electrochemical Properties and Challenges of Type II Silicon Clathrate Anode in Sodium Ion Batteries},
author = {Li, Xuemin and Steirer, K. Xerxes and Krishna, Lakshmi and Xiao, Chuanxiao and Fink, Kae and Santhanagopalan, Shriram},
abstractNote = {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.},
doi = {10.1149/2.1201913jes},
journal = {Journal of the Electrochemical Society},
number = 13,
volume = 166,
place = {United States},
year = {2019},
month = {9}
}

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Works referenced in this record:

Projector augmented-wave method
journal, December 1994


From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


A climbing image nudged elastic band method for finding saddle points and minimum energy paths
journal, December 2000

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