The reaction mechanism of SnSb and Sb thin film anodes for Na-ion batteries studied by X-ray diffraction, 119Sn and 121Sb Mössbauer spectroscopies

Loïc Baggetto, Hien Yoong Hah, Jean Claude Jumas, Charles E. Johnson, Jacqueline A. Johnson, Jong K. Keum, Craig A. Bridges, Gabriel M. Veith

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Abstract

The electrochemical reaction of Sb and SnSb anodes with Na results in the formation of amorphous materials. To understand the resulting phases and electrochemical capacities we studied the local order using 119Sn and 121Sb Mössbauer spectroscopies in conjunction with measurements performed on model powder compounds of Na-Sn and Na-Sb to further clarify the reactions steps. For pure Sb the sodiation starts with the formation of an amorphous phase composed of atomic environments similar to those found in NaSb, and proceeds further by the formation of crystalline Na3Sb. The reversible reaction takes place during a large portion of the charge process. At full charge the anode material still contains a substantial fraction of Na, explaining the lack of recrystallization into crystalline Sb. The reaction of SnSb yields Na3Sb at full discharge at higher temperatures (65 and 95 °C) while the RT reaction yields amorphous compounds. The electrochemically-driven, solid-state amorphization reaction occurring at RT is governed by the simultaneous formation of Na-coordinated Sn and Sb environments, as monitored by the decrease (increase) of the 119Sn ( 121Sb) Mössbauer isomer shifts. Overall, the monitoring of the hyperfine parameters enables to correlate changes in Na content to the local chemical environments.

Original languageEnglish
Pages (from-to)329-336
Number of pages8
JournalJournal of Power Sources
Volume267
DOIs
StatePublished - Dec 1 2014

Funding

This work was supported by the U.S. Department of Energy (DOE) , Basic Energy Sciences (BES) , Materials Sciences and Engineering Division (LB, GMV) . Microscopy research was supported via a user project supported by ORNL's Shared Research Equipment (ShaRE) User Program, which is also supported by DOE–BES. HYH, CEJ, JAJ would like to acknowledge the support of the Center for Laser Applications and the University of Tennessee Space Institute in relation with 121 Sb Mössbauer spectroscopy measurements. JCJ gratefully acknowledges Région Languedoc-Roussillon (France) for the financial support to the “X-rays and gamma-rays platform” of Université Montpellier II in relation with 119 Sn Mössbauer spectroscopy experiments.

Keywords

  • Antimony (Sb)
  • Sodium ion anode
  • Tin antimony (SnSb)
  • X-ray diffraction (XRD)

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